Dynamic photomask directed lithography based on electrically stimulated nematic liquid crystal architectures

Dynamic photomask directed lithography based on electrically stimulated nematic liquid crystal architectures | Research Square window.SnipcartSettings = { analytics: { enabled: false } }; (function() { var accessVector = localStorage.getItem('access_vector') || ''; window.dataLayer = window.dataLayer || []; if (accessVector) { window.dataLayer.push({ user: { profile: { profileInfo: { snid: accessVector } } } }); } })(); (function(w,d,s,l,i){w[l]=w[l]||[];w[l].push({'gtm.start':new Date().getTime(),event:'gtm.js'});var f=d.getElementsByTagName(s)[0],j=d.createElement(s),dl=l!='dataLayer'?'&l='+l:'';j.async=true;j.src='https://www.googletagmanager.com/gtm.js?id='+i+dl;f.parentNode.insertBefore(j,f);})(window,document,'script','dataLayer','GTM-K279D39R'); Browse Preprints In Review Journals COVID-19 Preprints AJE Video Bytes Research Tools Research Promotion AJE Professional Editing AJE Rubriq About Preprint Platform In Review Editorial Policies Our Team Advisory Board Help Center Sign In Submit a Preprint Cite Share Download PDF Article Dynamic photomask directed lithography based on electrically stimulated nematic liquid crystal architectures Lingling Shui, Mengjun Liu, Ruizhi Yang, Zhenghao Guo, Kexu Chen, and 5 more This is a preprint; it has not been peer reviewed by a journal. https://doi.org/ 10.21203/rs.3.rs-3992476/v1 This work is licensed under a CC BY 4.0 License Status: Published Journal Publication published 30 Oct, 2024 Read the published version in Nature Communications → Version 1 posted You are reading this latest preprint version Abstract Lithography technology is a powerful tool for preparing complex microstructures through projecting the patterns of static templates with permanent features onto samples. To simplify fabrication and alignment processes, dynamic photomask for multiple configurations preparation becomes increasingly noteworthy. Hereby, we report a dynamic photomask by assembling the electrically stimulated nematic liquid crystal (NLC) into multifarious architectures. We demonstrate that these architectures give rise to reconfigurable and switchable diffraction patterns via electrically modulating the hybrid phase arising from the NLC molecules. These electrically configurable diffraction patterns are adopted as metamask to produce multiple microstructures with height gradients in one-step exposure and hierarchical microstructures through multiple in-situ exposures using standard photolithography. The fabricated pattern has feature size about 3.2 times smaller than the electrode pattern and can be transferred onto silicon wafer via etching. This strategy can be extended to design diverse microstructures with great flexibility and controllability, offers a promising avenue for fabricating metamaterials via complex structures with simplified lithography processes. Physical sciences/Physics/Applied physics Physical sciences/Physics/Condensed-matter physics Physical sciences/Physics/Optical physics Figures Figure 1 Figure 2 Figure 3 Figure 4 Figure 5 Introduction The emergence of artificial metamaterial has opened new avenues for exploring the unusual electromagnetic, mechanical, optical and theological properties of the materials 1 – 4 . These artificial structures introduce a paradigm for engineering the materials with designable structural properties and thus enabling functions beyond the reach of existing bulky materials. They feature micron/nanoscale characteristics, which facilitates various applications ranging from hierarchical photonic devices 5 , 6 , electromagnetic and acoustic metamaterials 7 , 8 , mechanical metamaterials 9 , 10 , and thermal energy transfer 11 . So far, artificial structures have been primarily fabricated using lithography techniques, including two-photon lithography (TPL) 12 , electron beam lithography (EBL) 13 , nanoimprint lithography (NIL) 14 , capillary force lithography (CFL) 15 , and traditional three-dimensional (3D) printing 16 . Generally, TPL has the capability of producing high-resolution structures with feature size down to 200 nm 17 , 18 . However, similar to the EBL relying on pixel-by-pixel writing process 19 , the limited-throughput caused by seriality renders TPL time-consuming to pattern large-area microstructures 17 , 18 . Although this challenge can be partially mitigated by the high-throughput NIL and CFL which are particularly suitable for large-area patterning, they either heavily rely on the master imprint mold or lack flexibility in geometric design 14 , 20 , 21 . Alternatively, traditional 3D printing technique can offer great design flexibility, but it suffers from bottlenecks in patterning accuracy and inherent limitations in materials 22 . Generally, aforementioned lithography techniques either lean on static masks or have relatively low fabrication accuracy. In principle, the preparation of conventional artificial structures with single height gradient is relatively straightforward, whereas multi-height gradients should turn to top-down or bottom-up methods 23 – 26 . Hence, the cost-effective preparation method of hierarchical structures with micron/nanoscale features remains challenging. Traditionally, the fabrication of hierarchical structures based on static masks adopts multiple lithography processes requiring the successive replacement of different masks, which is sophisticated and challenging due to the difficulties in accurately aligning the patterns on the masks 13 , 27 – 29 . Although this challenge can be alleviated by employing multiplexed lithography, allowing for production of various multilevel microstructures, the fabrication of the mask remains complicated 30 . Recently, there has been an increasing attention on the temporal and spatial evolution facilitated by electrically stimulated liquid crystal (LC), as highlighted in these studies 31 , 32 . Nematic LC (NLC) stands out as a simple and versatile soft material characterized by optical birefringence and ability to assemble into multifarious architectures under the geometric confinement and external stimuli, thus generating dynamic diffraction patterns with designable properties 33 – 38 . Hence, these dynamic patterns are highly promising in photolithography as metamask for preparing structures with micron/nanoscale features onto the photosensitive materials through one-step lithography. Herein, we report a dynamic photomask for directed lithography, which is driven by diffraction pattern from assembling the electrically stimulated NLC molecules into multifarious architectures. The virtual metamasks are composed of reconfigurable and switchable diffraction patterns of the NLC architectures, which are enriched with information of grayscale and can be used as bridge in lithography. We adopt the Landau-de Gennes’s Q tensor and nonuniform finite difference method to theoretically predict the optical behavior of the NLC architectures under external stimuli. The resultant diffraction pattern, functioning as the metamask, successfully fabricates two-height gradients microstructure on negative photoresist (HN-018) using one-step lithography process, and the obtained microstructure has feature size about 3.2 times smaller than the initial electrode pattern. This also can produce hierarchical microstructure through in-situ manipulation of the working distance and simultaneous exposures. Moreover, the microstructure is transferred onto a silicon wafer through wet etching, yielding structures endowed with distinctive optical and mechanical properties that align with the diffraction pattern. Remarkably, our metamask is independent from incident wavelengths, making it compatible with a broad range of materials for lithography. This approach streamlines the controlled and flexible production of various microstructures, distinguishing itself through its simplicity, cost-effectiveness, and efficiency in manufacturing. The resulting multi-functional microstructures are highly advantageous for a multitude of applications. Results Principle of lithography utilizing metamask Figure 1 depicts the basic principle of the proposed dynamic photomask directed lithography. Figure. 1a and Supplementary Fig. 1 show the schematic setup to create the metamask based on the electrically stimulated assembly NLC molecules into architectures. The continuous-wave laser beam with working wavelength of 405 nm is expanded and then collimated by the lenses and aperture. The collimated beam is converted to circularly polarized light and then modulated by the NLC sample, generating coherent diffraction patterns that spatially evolve along the propagation direction (Fig. 1 a). The sample of the dynamic NLC photomask is consisted of uniaxial LC material (5CB, with positive dielectric anisotropy) sandwiched between a top substrate coated with uniform ITO and a bottom substrate with patterned ITO coated with a passivation layer (Hyflon) ( Supplementary Fig. 1 ). In principle, the optical axis of 5CB molecules undergoes constant fluctuations attributed to thermal movements, and hence only a small amount of energy is sufficient to reorient their directors. This remarkable characteristic allows for manipulating the NLC molecules with an external electric field. We calculate the molecular distributions (LC thickness: 50 µm) along the z -axis and x - z plane in response to the applied electric field (1 kHz, 400 Vpp) (Fig. 1 b and Supplementary Fig. 2 ). The NLC molecular directors tend to exhibit uniform state (90°) within the conductive ITO region, due to the uniform electric field distribution across the LC layer in the vertical direction (Fig. 1 b). On the contrary, in the circular aperture region without ITO, the NLC molecular directors with tilt angles varying from 33.23 to 90° are circularly symmetric in the transverse planes along z -axis, and follow the electric field in x-z plane, leading to a controllable phase profile. Consequently, when the laser beam passes through this region with specific phase retardation, typical diffraction patterns are generated (Fig. 1 a). Large quantity of complex diffraction patterns resulted from the constructive or destructive interference between neighboring patterns, appear in the propagation direction, thus providing a promising platform for photomask. The intensity distribution of one of the diffraction patterns is illustrated by the optical microscope (OM) image (Fig. 1 c). When it is employed as metamask to pattern photosensitive materials (negative photoresist HN-018), microstructure with 3D surface topography is obtained after one-step standard photolithographic process ( Fig. 1 d). Alternatively, we can also realize a new microstructure (Fig. 1 e) after transferring the pattern in Fig. 1 d to a silicon wafer by wet etching, providing a promising technique for microelectromechanical systems (MEMS). Modulation of diffraction patterns We firstly simulate the optical performance of the NLC architectures under the stimulation of electric field after efficiently calculating the molecular director configuration in Fig. 1 b. Here, typical parameters of a circle electrode pattern are given as follows: diameter of the electrode ( D = 20.11 µm), spacing between neighboring electrode patterns ( L = 19.89 µm), and thickness of LC layer ( H = 50 µm). The working wavelength of the incident continuous-wave laser beam is 405 nm. The driving alternating voltage (AC) of square wave is set at a frequency of 1 kHz and 400 peak-to-peak value (Vpp) 39 , 40 . Figure 2 a (Ⅰ) shows the simulated images of diffraction patterns propagating along the z -axis at specific distance: z = 0, 335.0, 1401.0, 3188.0, and 4176.0 µm. The diffraction pattern on the LC layer surface is determined to be z = 0 µm, taking the shape of circle. As z increases, diverse diffraction patterns with different complexity appear within the circular aperture, morphing from flower-like shapes at z = 335.0 µm to squares and ultimately backed to circles in a cyclic manner. Correspondingly, we experimentally record the OM images of diffraction patterns at z = 85.3, 419.9, 1485.0, 3250.0, and 4194.9 µm, which are consistent with the simulation results (Fig. 2 a (Ⅱ) ). We also provide two movies to illustrate the dynamic evolution of diffraction patterns in the simulation and experiment ( Supplementary Movies 1 and 2 ). These movies show that the diffraction patterns repeat themselves along the propagation direction after a regular distance away from the exit plane, following the theory of Talbot effect 41 . This regular distance is widely known as Talbot length and given by \(Z=2\left( {{{{d^2}} \mathord{\left/ {\vphantom {{{d^2}} \lambda }} \right. \kern-0pt} \lambda }} \right)\) , where d is a pitch ( \(d=D+L\) ) and λ is the incident wavelength. Since the image at \({{{d^2}} \mathord{\left/ {\vphantom {{{d^2}} \lambda }} \right. \kern-0pt} \lambda }\) corresponds to a negative image, thus we can simply consider half of the Talbot length as the periodic length ( \({Z_{\text{T}}}={{{d^2}} \mathord{\left/ {\vphantom {{{d^2}} \lambda }} \right. \kern-0pt} \lambda }\) ) to avoid the repetition of optical patterns. The simulated and experimental \({Z_{\text{T}}}\) values are estimated to be 4176.0 and 4194.9 µm, indicating a good match, whereas the theoretical \({Z_{\text{T}}}\) value is 3950.6 µm based on the assumptions of working wavelength of 405 nm and a pitch of 40 µm. This minor difference between the simulated and theoretical values can be attributed to the lack of consideration for the cell thickness in the calculation. The simulated \({Z_{\text{T}}}\) value includes the propagation distance between the LC layer and the glass and air. Moreover, it can be observed that \({Z_{\text{T}}}\) is inversely proportional to the wavelength, implying that the dynamic change of diffraction pattern can be tuned with the wavelength. When the wavelength is 532 nm, \({Z_{\text{T}}}\) value is shortened by 0.76 times (Fig. 2 a (III) ). However, the same diffraction patterns can be obtained at z = 0.9, 319.0, 1111.0, 2470.0, and 3210.0 µm. This helps to demonstrate that the sample is broadband, which is a significant advantage of the NLC photomask for lithography, due to the greatly expanding selection range of photosensitive materials. To compare the patterns under different conditions, a dimensionless ratio R applicable throughout the entire study is defined as \({Z \mathord{\left/ {\vphantom {Z {{Z_{\text{T}}}}}} \right. \kern-0pt} {{Z_{\text{T}}}}}\) . The pluralistic morphology of the diffraction pattern can also be modulated by changing the electrode shapes ( Supplementary Fig. 3 ). Moreover, it is very reasonable to infer that the diffraction pattern can also be tuned by the electrode parameters. This is demonstrated by the experiments in Supplementary Fig. 4a , where two samples ( D = 29.87, L = 10.13 µm and D = 35.05, L = 5.95 µm) with the same pitch but different L and D are fabricated and optically characterized. In order to better illustrate the properties of diffraction pattern, we plot the normalized intensity of gray value on a representative line. The intensity in the selected yellow dashed line in the OM images reveals that the diffraction patterns contain four gray levels, four peaks and valleys when D = 29.87 and L = 10.13 µm (Fig. 2 b). The gray levels represent the gradients, and the peak or valley along the x -axis reflects an indicator of microstructure. However, the features increase to five and six when D = 35.05 and L = 5.95 µm. This is because the small deflection angle (28.20°) of the electrically stimulated NLC molecules can lead to maximum refraction of light ( Supplementary Fig. 4b ), resulting in an increase of interference intensity between the neighboring the electrode patterns when D = 35.05 and L = 4.95 µm. Compared to the case of D = 29.87 and L = 10.13 µm with a minimum angle of 30.49°, the thickness of the electrically stimulated NLC molecules is also increasing, which plays a synergistic role in the complexity of diffraction patterns ( Supplementary Fig. 4b ). Therefore, it is also imperative to delve into exploring how LC layer thickness affects the gray levels of diffraction patterns when the D and L remain unchanged. As aforementioned in Fig. 1 b, the orientations of the NLC molecules experience sufficiently perturbations when the LC thickness falls below 9 µm when D = 20.11 and L = 19.89 µm. The normalized intensity (Fig. 2 c) along the designated black dashed line in the simulated diffraction pattern ( Supplementary Fig. 5a ), showcases discernible variations corresponding to different LC layer thickness ( H = 1, 5, 9, 30, 50 µm). At a thickness of 1 µm, the intensity remains a fixed value out nuanced gradients of gray levels. However, three distinct gray levels emerge with a relatively low contrast at a LC thickness of 5 µm. When the LC thickness is beyond 9 µm, the diffraction pattern characterized by pronounced contrast remains virtually unaltered. This phenomenon can be attributed to the vertical alignment of NLC molecules near the upper electrode, and thus there is an absence of birefringence, leading to negligible impact on the diffraction pattern. Moreover, owing to the small extinction coefficient of 5CB 42 , the transmitted light intensity exhibits remarkable stability even the LC thickness reaching 50 µm. Simultaneously, these experimentally captured diffraction patterns adopt consistently aligned when H = 30, 50, 80, and 100 µm ( Supplementary Fig. 5b ). Moreover, we also investigate the other electrode parameter and find that the diffraction patterns are highly adjustable ( Supplementary Fig. 6 ). Although these diffraction patterns are reconfigurable, they are periodic and follow the Talbot length. Figure 2 d shows the corresponding \({Z_{\text{T}}}\) values as a function of the square pitch d . A linear correlation of \({Z_{\text{T}}}=2.47{d^2}+190.79\) ( R 2 = 0.99) can be observed in the range of 25 − 80 µm. Similarly, the \({Z_{\text{T}}}\) values match excellently with the same pitch of 40 µm when the electrode shapes are circular, octagonal, hexagonal, square, and triangular apertures in the red dashed line of Fig. 2 c. Supplementary Fig. 5c also shows the \({Z_{\text{T}}}\) values remain nearly constant at different LC layer thickness, with the slight discrepancies attributed to the variations in LC layer thickness. The cyclic periodicity of the diffraction pattern in the direction of light propagation allows for greatly selecting metamask for lithography. Fabrication of microstructure The efficiency of lithography and stability of photomask are two crucial factors in practical application. In this study, the applied electric field requires certain relaxation time to trigger the rotation of NLC molecules towards the state of minimum total free energy. The measured native response on-time is 477 ms following the case with 400 Vpp (Fig. 3 a). Subsequently, upon deactivating the electric field, the NLC molecules revert to their original state within a timeframe of 480 ms. This response time is at least four orders of magnitude smaller than the entire lithography process, proving that our proposal is efficient enough for lithography. Furthermore, the OM images in Fig. 3 a affirm that the transitions between stable configurations are entirely reversible, maintaining ultrahigh stability even after 100 switching cycles. Hence, the assembled NLC architectures, functioning as a photomask generator, have the advantages of fast response, excellent stability, and outstanding repeatability, rendering them exceptionally well-suited for the fabrication of microstructure for active applications. In our strategy, the diffraction patterns formed by NLC architectures contain gray information, which can serve as gray mask to pattern the multi-height gradient microstructure. Although microstructures featuring multi-height gradients have been widely utilized in fields such as optics and surface engineering 3 , 43 , efficient fabrication remains a challenge. Here, we prove the feasibility of using this gray mask to prepare a typical multi-height gradient microstructure through one-step lithography. We choose the diffraction pattern of sample with circular electrode array ( d = 40 µm, H = 50 µm) at position of 1060 µm (Fig. 3 b). The normalized intensity of the dashed line in the simulated diffraction pattern exhibits a minimum 6 gray levels ( Supplementary Fig. 7 ). Each peak or valley along the x -axis reflects an indicator of lithographic resolution, with simulation results suggesting an achievable resolution of 1.2 µm. After using this diffraction pattern (Fig. 3 c) as a metamask for lithography, the diffraction pattern is successfully replicated onto the negative HN-018 photoresist coated on the glass by one-step lithography, which can be partially demonstrated by the 2D profile image of microstructure (Fig. 3 d). The resulting 3D surface topography image displays at least two-height gradients on photosensitive materials with an 8 µm thickness (Fig. 3 e). The 1st gradient microstructure corresponds to the glass substrate, as evidenced by the region with null diffraction light. The average size measures 6.2 µm, which is 3.2 times smaller than the designed electrode size, as shown in the red dotted box in Fig. 3 e. The 2nd gradient microstructure displays a thickness ranging between 4 and 6 µm, while the 3rd gradient manifests a thickness of approximately 8 µm, aligning with the initial thickness of the photoresist layer. Figure 3 f plots the normalized intensity and height of the selected dashed line containing 3 levels on the image of Figs. 3 c,e. The 2nd level has subtle difference within a range, attributing to the low accuracy of laser. This approach for fabricating multi-height gradient microstructures through one-step lithography is time-saving and cost-effective. Owing to the high freedom of this photomask, hierarchical microstructures could also be easily generated in-situ using the one-step multilayer photolithography technique. Specifically, the sample undergoes exposure to the first target light field and then to the second light field at another longitudinal location, both originating from the same photomask (Fig. 4 a). Through this process, the two light fields are superimposed and embedded together into the same sample, hence the hierarchical microstructure can be realized through rather simple lithography process. Theoretically, holographic image through incorporation of multiple into the same hierarchical 3D microstructure can be achieved by multi-exposing process (Fig. 4 a). As a proof of concept, we experimentally fabricate a hierarchical microstructure by superimposing two metamask, namely two diffraction patterns (Fig. 4 b). The sample of HN-018 photoresist coated on glass is initially exposed at z = 3400 µm and then mechanically moved to 4100 µm for second exposure. Ultimately, three levels microstructure is achieved after developing. The 3D surface topography image of resultant hierarchical microstructure shows that the 1st level microstructure corresponds to the glass substrate, the 2nd level microstructure is formed by the first exposure, and the 3rd level microstructure emerges from the combining effects of the two exposures, resulting in the highest gradients (Fig. 4 c). It should be emphasized that the dynamic photomask for lithography facilitates the creation of hierarchical microstructures in a novel manner, avoiding alignment errors that may arise in multiple lithography compared to EBL 13 . Naturally, the realization of single-layer microstructure on the photosensitive material (HN-018) photoresist coated on the silicon wafer is possible through using our metamask (Fig. 5 a). The recorded 3D surface topography image after lithography aligns closely with the OM image (Fig. 5 b). Subsequently, leveraging the derived 3D surface topography of microstructure, the mechanical performance of the obtained material is calculated under the 5×10 8 N/m 2 stress using the open-source COMSOL software (Fig. 5 b). It is found that the microstructure is anisotropic and possesses a period of 180°. Such kind of anisotropic microstructural materials plays a key role in areas such as the human brain or tendons 10 . Apart from the demonstration of producing anisotropic microstructure, we transfer the resultant microstructures from the photosensitive material to the silicon wafer by a wet etching process (12.5 wt% TMAH, 300 rpm, 80 ℃, 5 min). The scanning electron microscopy (SEM) image of the produced microstructure (Fig. 5 c) illustrates that there is bowl-like structure from a similar square master microstructure, characterized by numerous random upright pyramids (UPs) on the surface. In contrast, the numbers of UPs on the surface decrease in case without microstructure under the same experiment condition ( Supplementary Fig. 8 ). It has been already proved that these textured surfaces which are covered by UPs are promising for manufacturing high-efficiency silicon solar cells 44 , 45 . As depicted in Figs. 5 d,e, the reflectance spectrum shows that when the standard silicon wafer as a baseline is thought 100%, the overall average reflectance of the textured surfaces covered with UPs but that without trapping of microstructure is 60%. In contrast, the overall average reflectance can reduce 19%, because the trapping effects of microstructure can be generally understood by the multiple reflection that maximizes the absorption of the incident light. It implies that the microstructures can be transferred onto the silicon wafer, holding the promising in the high-efficiency solar energy harvesting. Discussion We have developed a cost-saving methodology of harnessing electrically driven NLC assembly architectures to craft a dynamic photomask. Our study demonstrates that modulating the spatially localized orientations of the NLC molecules enables the tuning of the wavefront of the incident laser beam, and consequently leads to intricate diffraction patterns. These diffraction patterns are enriched with grayscale information, which may function as metamask and serve as powerful catalysts for lithography. We successfully prepare the multi-height gradients microstructure onto photosensitive materials (HN-018) by using our proposed metamask. Furthermore, based on the high freedom of the photomask in the propagation direction owing to the coherence between neighborhood electrode patterns, we achieve a kind of hierarchical microstructures through in-situ modulation of work distance from sample photomask. In comparison with the traditional multilayered photolithography methods for fabricating hierarchical microstructures, our proposal eliminates intermediate alignment steps and significantly enhances the efficiency. Remarkably, the microstructure can be transferred onto silicon wafer, and the ensuing microstructures featuring random upright pyramid shapes showcase good optical performance, expanding the application of this methodology. However, we notice in the experiment that the resolution and height gradient of the obtained microstructures deviated from perfection in comparison to the simulation. Envision an enhancement in our work, enhancing the uniformity and power output of the laser, reducing the pattern size, or using high-power ultraviolet laser will lead to better precision, more height gradients and even nanoscale structures. Furthermore, the established simulation method serves as a valuable predictive tool, successfully forecasting a spectrum of diffraction patterns. Looking forward, our vision encompasses the capability to create arbitrary multilevel structures even holographic image through the pre-superimposition of meticulously designed patterns. These strides open expansive application possibilities for customizable metamaterials across various fields such as mechanics, optics, photonics, electricity and so on. Materials and methods Experimental design of photomask We fabricated the electrode arrays using a standard lithography process. Initially, the ITO substrate was cleaned with a 4 wt% alkaline solution, followed by rinsing with DI water and drying with nitrogen blowing. A positive-type photoresist (SUN-120P) was spin-coated (step 1: 500 rpm for 5 s; step 2: 3000 rpm for 60 s) onto ITO substrate and then soft-baked at 120 ℃ for 90 s on the hot plate (EH20B, Lab Tech, Beijing, China). UV light exposure (13 mW·cm − 2 for 13 s) was performed using an aligner (URE-2000/35, Institute of Optics and Electronics, Chengdu, China) with a chrome mask with designed patterns, and then the substrates were submerged in a developer (0.5 wt% KOH) for 90 s. Afterwards, it was cleaned with DI water and blow dried with nitrogen. The patterned photoresist was then hard-baked on the hot plate at 120°C for 30 min. The substrates were then submerged in an acidic etchant (37 wt% HCl: 68 wt% HNO 3 : H 2 O = 50: 3: 50, V/V) until the exposed ITO area was fully etched. The photoresist residue was removed by ethanol after cleaned by DI water and then dried by nitrogen blow to obtain the patterned electrode. The LC materials were assembled between two glass substrates ( Supplementary Fig. 1 ). First, the bare and patterned ITO electrode was spin-coated with Hyflon (377 nm) to form a stable dielectric protective layer. The upper substrate was made of a Hyflon-coated uniform ITO electrode. The lower substrate was patterned electrode with Hyflon. The cell was assembled by patterned electrode and a bare ITO electrode using a commercial double tape as a spacer. To easily connect the wires, two substrates were controlled in dislocation. Subsequently, the LC cell was filled with 5CB by capillary force at 40°C above the isotropic temperature and then cooled down to the room temperature. Additionally, we sealed the edge using the UV curing to prevent the leakage of LC. Schematic diagram of optical path Supplementary Fig. 1 depicts the experimental platform to optically characterize the samples. A collimated Gaussian beam is expanded by the beam expander consisting of lens1, pinhole and lens2. After that, it is converted into circularly polarized light by a linear polarizer (LP) and a quarter waveplate (QWP). Finally, the collimated beam reflected by a mirror normally impinges onto the sample placed on the microscope stage. Charge Coupled Device (CCD, Leica DMC 4500) together with a ×5 magnification objective lens is used to collect the diffraction field of the sample. The blue double arrow represents the moving direction of the stage, and the distance between the surface of NLC layer and the acquired OM image is defined as “ z ” ( Supplementary Fig. 1 ). The diameter and spacing of the patterned electrode are denoted with “ D and L ” and the pitch is “ \(d=D+L\) ”. The thickness of LC layer is described as “ H ”. Preparation of lithography samples The microscope cover glass and the silicon wafer were cleaned by soaking it in piranha solution (H 2 O 2 : H 2 SO 4 = 1: 3), and then rinsed with DI water and blow dried using the nitrogen. The HN-018 photoresist was spin-coated on the glass and silicon wafer: step 1: 500 rpm for 5 s, step 2: 1000 rpm for 65 s for 8 µm thickness, step 1: 500 rpm for 5 s, step 2: 2000 rpm for 65 s for 4 µm thickness, and step 1: 500 rpm for 5 s, step 2: 2500 rpm for 65 s for 3 µm thickness. After that, it was soft-baked at 90 ℃ for 90 s, exposed, developed for 30 s with 0.4 wt% KOH, and then hard-baked at 210 ℃ for 30 min on a hot plate. Numerical methods To simulate the optical properties of the NLC device, the first task is to efficiently calculate the molecular director configuration. According to P. G. de Gennes 46 , the average molecule direction of rod-shaped uniaxial molecule 5CB can be described by its director n ( n = - n ). Therefore, the Landau-de Gennes’s Q tensor is employed to represent the director’s configuration and the elastic free energy of NLC. Afterwards, the NLC molecular directors tend to rotate to reduce the overall energy of the system and ultimately rearrange along the electric field lines based on the dielectric anisotropy when a voltage is applied. The total free energy is minimized when the energy of the electric field is competitive with the elastic energy of NLC. The Euler-Lagrange equations are used to solve the director configuration by using the relaxation method based on dynamics 47 . To expedite the calculation process, techniques such as the momentum gradient descent algorithm, the improved successive over relaxation method, the multigrid, and the symmetric boundary conditions are utilized. The formulas of calculation processes refer to the supporting information . After obtaining the director configuration of NLC molecules between the sandwich electrodes, this information is used to model the device and then simulate the diffraction field using the commercial-available FDTD (Finite-Difference Time-Domain) software. Basically, the model in this study cannot be fully simulated by the FDTD software, due to the heavy computational cost. However, we notice that the light passing through the NLC layer propagates through a uniform and parallel medium of glass and air. In this case, the diffraction pattern can be efficiently simulated using the vectorial Rayleigh-Sommerfeld diffraction formula and fast Fourier transform, which help to greatly reduce the computing resources and run time. Materials Indium-tin-oxide (ITO) coated glass (700 µm, 90 ± 10 Ω·sq − 1 , Leaguer Optronics CO., Ltd, Shenzhen, China) was employed as electrode substrates. The 110 µm thickness microscope cover glass (Fisherbrand®) was procured by Thermo Fisher scientific, Germany. P-type (100) 4″ silicon wafers were acquired from Lijing Optoelctronics Co., Ltd. (Suzhou, China). Nematic liquid crystal of 4-cyano-4’-pentyl-biphenyl (5CB, T NI = 35 ℃; K 11 = 6.2, K 22 = 3.9, K 33 = 8.2 pN; ε ‖ = 18.5, ε ⊥ = 7.0; n e = 1.6975, n o = 1.5350) was purchased from J&K Scientific Co., Ltd., China. Hyflon (AD 40 SX 2.5 wt%) was obtained from Solvay (Shanghai) Co., Ltd., China. A negative-type photoresist (HN-018) and positive-type photoresist (SUN-120P) was soured from Suntific Microelectronic Materials Co. Ltd, Weifang, China. KOH and TMAH (Tetramethylammonium hydroxide) were purchased from Aladdin, Shanghai, China. H 2 O 2 , H 2 SO 4 , HCl and HNO 3 was obtained Guangzhou chemical reagent Co., Ltd., Guangzhou, China. Declarations Data availability: All data are available in the main text or the Supplementary materials. Acknowledgments: We acknowledge all lab members for supporter and guidance on this project. We thank Minxing Lu for the characterization of 3D surface topography. We appreciate the financial support from the Special Project for Marine Economy Development of Guangdong Province (GDNRC[2023]26), the Key Project of National Natural Science Foundation of China (No. 12131010), the International Cooperation Base of Infrared Reflection Liquid Crystal Polymers and Device (2015B050501010), Guangzhou Basic and Applied Basic Research Project (202201010531) and the Science and Technology Project of South China Normal University (21KJ05). Author contributions: M.L., R.Y., H.Y. and L.S. proposed and designed all experiments. M.L., R.Y., K.C., H.F., H.L., S.H., H.Y. and L.S. performed the experiments. M.L., R.Y., Z.G., K.C., H.F., H.L., S.H., M.Z., H.Y. and L.S. discussed and analyzed the experimental results as well as the presentation of the results. M.L., Z.G. and H.Y. contributed to the numerical simulation work. M.L., H.F., K.C., H.L., M.Z. and L.S. participated the discussion. M.L., R.Y., H.Y. and L.S. wrote and polished the initial manuscript. All authors took part in formulating and writing toward the finalization of the manuscript. Competing interests: All other authors declare that they have no competing interests. References Kim, T., Bae J.-Y., Lee, N. & Cho, H. H. Hierarchical metamaterials for multispectral camouflage of infrared and microwaves. Adv. Funct. Mater. 29 , 1807319 (2019). Zhang, H., Wu, J., Fang, D. & Zhang, Y. Hierarchical mechanical metamaterials built with scalable tristable elements for ternary logic operation and amplitude modulation. Sci. Adv. 7 , eabf1966 (2021). Xie, Y.-Y. et al . Metasurface-integrated vertical cavity surface-emitting lasers for programmable directional lasing emissions. Nat. Nanotechnol . 15 , 125-131 (2020). Run, H. et al. Thermal camouflaging metamaterials. Mater. Today . 45 , 120-141 (2021). Murataj, I. et al. Hyperbolic metamaterials via hierarchical block copolymer nanostructures. Adv. Opt. Mater . 9 , 2001933 (2021). Balli, F., Sultan, M., Lami, S. K. & Hastings, J. T. A hybrid achromatic metalens. Nat. Commun . 11 , 3892 (2020). Feng, X. et al. Hierarchical metamaterials for laser-infrared-microwave compatible camouflage. Opt. Express . 28 , 9445-9453 (2020). Weiner, M., Ni, X., Li, M., Alu, A. & Khanikaev, A. B. Demonstration of a third-order hierarchy of topological states in a three-dimensional acoustic metamaterial. Sci. Adv . 6 , eaay4166 (2020). Dudek, K. K., Martinez, J. A. I., Ulliac, G. & Kadic, M. Micro-scale auxetic hierarchical mechanical metamaterials for shape morphing. Adv. Mater . 34 , 2110115 (2022). Yu, X., Zhou, J., Liang, H., Jiang, Z. & Wu, L. Mechanical metamaterials associated with stiffness, rigidity and compressibility: A brief review. Prog. Mater. Sci . 94 , 114-173 (2018). Wang, K., Lin, F., Chen, J., Wei, Z., Wei, K. & Yang X. Three-dimensional hierarchical metamaterials incorporating multi-directional programmable thermal expansion. Mech. Mater. 163 , 104095 (2021). Gan, Z., Cao, Y., Evans, R. A. & Gu, M. Three-dimensional deep sub-diffraction optical beam lithography with 9 nm feature size. Nat. Commun . 4 , 2061 (2013). Yoon, G., Kim, I., So, S., Mun, J., Kim, M. & Rho, J. Fabrication of three-dimensional suspended, interlayered and hierarchical nanostructures by accuracy-improved electron beam lithography overlay. Sci. Rep . 7 , 6668 (2017). Ofir, Y., Moran, I. W., Subramani, C., Carter, K. R. & Rotello, V. M. Nanoimprint lithography for functional three-dimensional patterns. Adv. Mater. 22 , 3608-3614 (2010). Li, H., Yu, W., Xu, J., Yang, C., Wang, Y. & Bu, H. Hierarchical structure formation and pattern replication by capillary force lithography. RSC Adv . 4 , 39684-39690 (2014). Zhou, X. & Liu, C.-J. Three-dimensional printing for catalytic applications: current status and perspectives. Adv. Funct. Mater . 27 , 1701134 (2017). Kawata, S., Sun, H. B., Tanaka, T. & Takada, K. Finer features for functional microdevices - Micromachines can be created with higher resolution using two-photon absorption. Nature 412 , 697-698 (2001). Harinarayana, V. & Shin, Y. C. Two-photon lithography for three-dimensional fabrication in micro/nanoscale regime: A comprehensive review. Opt Laser Technol . 142 , 107180 (2021). Myers, B. D. & Dravid, V. P. Variable pressure electron beam lithography (VP- e BL): A new tool for direct patterning of nanometer-scale features on substrates with low electrical conductivity. Nano Lett . 6 , 963-968 (2006). Guo, L. J. Nanoimprint lithography: methods and material requirements. Adv. Mater . 19 , 495-513 (2007). Cai, Y., Zhao, Z., Chen, J., Yang, T. & Cremer, P. S. Deflected capillary force lithography. ACS Nano 6 , 1548-1556 (2012). Ligon, S. C., Liska, R., Stampfl, J., Gurr, M. & Muelhaupt, R. Polymers for 3D printing and customized additive manufacturing. Chem. Rev . 117 , 10212-10290 (2017). Chen, Y., Yang, X. & Gao, J. 3D Janus plasmonic helical nanoapertures for polarization-encrypted data storage. Light Sci. Appl . 8 , 45 (2019). Ko, T.-J. et al. Single-step plasma-induced hierarchical structures for tunable water adhesion. Sci. Rep . 10 , 874 (2020). Eckel, Z. C., Zhou, C., Martin, J. H., Jacobsen, A. J., Carter, W. B. & Schaedler, T. A. Additive manufacturing of polymer-derived ceramics. Science 351 , 58-62 (2016). Aubert, T., Huang, J.-Y., Ma, K., Hanrath, T. & Wiesner, U. Porous cage-derived nanomaterial inks for direct and internal three-dimensional printing. Nat. Commun . 11 , 4695 (2020). Liu, N., Guo, H., Fu, L., Kaiser, S., Schweizer, H. & Giessen, H. Three-dimensional photonic metamaterials at optical frequencies. Nat. Mater . 7 , 31-37 (2008). Xu, X. et al. Multiple-patterning nanosphere lithography for fabricating periodic three-dimensional hierarchical nanostructures. ACS Nano 11 , 10384-10391 (2017). Choi, S. & Park, J.-K. Two-step photolithography to fabricate multilevel microchannels. Biomicrofluidics 4 , 046503 (2010). Cho, H. et al. Multiplex lithography for multilevel multiscale architectures and its application to polymer electrolyte membrane fuel cell. Nat. Commun . 6 , 8484 (2015). Clerc, M. G., Kowalczyk, M. & Zambra, V. Topological transitions in an oscillatory driven liquid crystal cell. Sci. Rep . 10 , 19324 (2020). Li, Y.-L. et al. Tunable liquid crystal grating based holographic 3D display system with wide viewing angle and large size. Light Sci. Appl . 11 , 188 (2022). Park, J., Won, K. & Kim, Y. Liquid crystal between two distributed Bragg reflectors enables multispectral small-pitch spatial light modulator. Light Sci. Appl . 11 , 210 (2022). Kim, D. S., Copar, S., Tkalec, U. & Yoon, D. K. Mosaics of topological defects in micropatterned liquid crystal textures. Sci. Adv . 4 , eaau8064 (2018). Yuan, Y., Liu, Q., Senyuk, B. & Smalyukh, I. I. Elastic colloidal monopoles and reconfigurable self-assembly in liquid crystals. Nature 570 , 214-218 (2019). Zola, R. S., Bisoyi, H. K., Wang, H., Urbas, A. M., Bunning, T. J. & Li, Q. Dynamic control of light direction enabled by stimuli-responsive liquid crystal gratings. Adv. Mater . 31 , 1806172 (2019). Peddireddy, K., Copar, S., Le, K. V., Musevi, I., Bahr, C. & Jampani, V. S. R. Self-shaping liquid crystal droplets by balancing bulk elasticity and interfacial tension. Proc. Natl. Acad. Sci. U.S.A . 118 , e2011174118 (2021). Ni, J. et al. Three-dimensional chiral microstructures fabricated by structured optical vortices in isotropic material. Light Sci. Appl . 6 , e17011 (2017). Kamal, W. et al. Spatially patterned polymer dispersed liquid crystals for image-integrated smart windows. Adv. Opt. Mater . 10 , 2101748 (2022). Shin, Y., Jiang, J., Qin, G., Wang, Q., Zhou, Z. & Yang, D.-K. Patterned waveguide liquid crystal displays. RSC Adv . 10 , 41693-41702 (2020). Rodrigues, J. S., Mendes, C. V. C., Fonseca, E. J. S. & Jesus-Silva, A. J. Talbot effect in optical lattices with topological charge. Opt. Lett . 42 , 3944-3947 (2017). Pan, R.-P., Hsieh, C.-F., Pan, C.-L. & Chen, C.-Y. Temperature-dependent optical constants and birefringence of nematic liquid crystal 5CB in the terahertz frequency range. J. Appl. Phys . 103 , 093523 (2008). Zheng, H., Zhou, Y., Ugwu, C. F., Du, A., Kravchenko, I. I. & Valentine, J. G. Large-scale metasurfaces based on grayscale nanosphere lithography. ACS Photonics 8 , 1824-1831 (2021). Chen, H. et al. Vertically aligned InGaN nanowire arrays on pyramid textured Si (100): A 3D arrayed light trapping structure for photoelectrocatalytic water splitting. Chem. Eng. J. 406 ,126757 (2021). Tong, R., Li, C., Ma, S., Liu, X., Zou, S. & Liu, D. Upright pyramids vs. inverted pyramids surface textures: a comparative investigation on the electrical properties of PERC solar cells. J. Mater. Sci. Mater. Electron. 34 , 54 (2023). Gennes, P. G. & Prost, J. The Physics of Liquid Crystals (Oxford Univ. Press, Oxford, 1993). Xiong, J., Chen, R. & Wu, S.-T. Device simulation of liquid crystal polarization gratings. Opt. Express . 27 , 18102-18112 (2019). Additional Declarations There is NO Competing Interest. There is no conflict of interest Supplementary Files Supplementaryinformation.pdf Supplementary information SupplementaryMovies.rar Supplementary Movies Cite Share Download PDF Status: Published Journal Publication published 30 Oct, 2024 Read the published version in Nature Communications → Version 1 posted You are reading this latest preprint version Research Square lets you share your work early, gain feedback from the community, and start making changes to your manuscript prior to peer review in a journal. As a division of Research Square Company, we’re committed to making research communication faster, fairer, and more useful. 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Also discoverable on Platform About Our Team In Review Editorial Policies Advisory Board Help Center Resources Author Services Accessibility API Access RSS feed Manage Cookie Preferences © Research Square 2026 | ISSN 2693-5015 (online) Privacy Policy Terms of Service Do Not Sell My Personal Information {"props":{"pageProps":{"initialData":{"identity":"rs-3992476","acceptedTermsAndConditions":true,"allowDirectSubmit":false,"archivedVersions":[],"articleType":"Article","associatedPublications":[],"authors":[{"id":275421609,"identity":"ce64cc6e-08d1-4d6c-895b-6a01130878f7","order_by":0,"name":"Lingling Shui","email":"data:image/png;base64,iVBORw0KGgoAAAANSUhEUgAAAZAAAAAyAQMAAABI0h/eAAAABlBMVEX///8AAABVwtN+AAAACXBIWXMAAA7EAAAOxAGVKw4bAAAAzElEQVRIiWNgGAWjYDACCQaGAw8KbOB8xgaitCQYpJGohSHB4DAJWuRn9xgCbTkfzcB/+NljHgYb2Q0HmJ89wKfF4M4ZA6CW27kNEmnmxjwMacYbDrCZG+DVIpED08LDJs3DcDhxwwEeNgm8DpsB1nIut4H/DEjLf8JaGG6AtRzIbWDIAWk5QFiLwY20AqCW5Nw2iTQzyTkGycYzD7OZEXBY8uYPHyrscvuBISbxpsJOtu948zP8DoMBNoilQMxMlPpRMApGwSgYBfgAAHUjRWVfmrw8AAAAAElFTkSuQmCC","orcid":"https://orcid.org/0000-0001-5976-1355","institution":"South China Normal University","correspondingAuthor":true,"prefix":"","firstName":"Lingling","middleName":"","lastName":"Shui","suffix":""},{"id":275421610,"identity":"29859d78-1331-4c98-9202-86adff8c6459","order_by":1,"name":"Mengjun Liu","email":"","orcid":"","institution":"South China Normal University","correspondingAuthor":false,"prefix":"","firstName":"Mengjun","middleName":"","lastName":"Liu","suffix":""},{"id":275421611,"identity":"d58a6d47-7a30-4013-9549-483c2343e082","order_by":2,"name":"Ruizhi Yang","email":"","orcid":"","institution":"South China Normal University","correspondingAuthor":false,"prefix":"","firstName":"Ruizhi","middleName":"","lastName":"Yang","suffix":""},{"id":275421612,"identity":"2b893fad-c80e-4cc2-abc0-b5fdac864a87","order_by":3,"name":"Zhenghao Guo","email":"","orcid":"","institution":"South China Normal University","correspondingAuthor":false,"prefix":"","firstName":"Zhenghao","middleName":"","lastName":"Guo","suffix":""},{"id":275421613,"identity":"a9ce47f6-6125-4278-9a39-6593e05bb60c","order_by":4,"name":"Kexu Chen","email":"","orcid":"","institution":"South China Normal University","correspondingAuthor":false,"prefix":"","firstName":"Kexu","middleName":"","lastName":"Chen","suffix":""},{"id":275421614,"identity":"49684bdd-78f3-4eac-a848-bd26e817d062","order_by":5,"name":"Haoqiang Feng","email":"","orcid":"","institution":"South China Normal University","correspondingAuthor":false,"prefix":"","firstName":"Haoqiang","middleName":"","lastName":"Feng","suffix":""},{"id":275421615,"identity":"bc432420-65ca-462b-afd4-c070e6cb35ef","order_by":6,"name":"Han Lu","email":"","orcid":"","institution":"South China Normal University","correspondingAuthor":false,"prefix":"","firstName":"Han","middleName":"","lastName":"Lu","suffix":""},{"id":275421616,"identity":"3c1cd77d-3a96-4d67-8baf-dc3bc29a5c96","order_by":7,"name":"Shijian Huang","email":"","orcid":"","institution":"South China Normal University","correspondingAuthor":false,"prefix":"","firstName":"Shijian","middleName":"","lastName":"Huang","suffix":""},{"id":275421617,"identity":"ca5bb165-3e34-4ac0-8c0b-816ed2e12de4","order_by":8,"name":"Minmin Zhang","email":"","orcid":"","institution":"South China Normal University","correspondingAuthor":false,"prefix":"","firstName":"Minmin","middleName":"","lastName":"Zhang","suffix":""},{"id":275421618,"identity":"0b2ee05c-7933-41a6-b74f-eb2e58dd6b4a","order_by":9,"name":"Huapeng Ye","email":"","orcid":"https://orcid.org/0000-0001-8472-8434","institution":"South China Normal University","correspondingAuthor":false,"prefix":"","firstName":"Huapeng","middleName":"","lastName":"Ye","suffix":""}],"badges":[],"createdAt":"2024-02-27 02:15:33","currentVersionCode":1,"declarations":"","doi":"10.21203/rs.3.rs-3992476/v1","doiUrl":"https://doi.org/10.21203/rs.3.rs-3992476/v1","draftVersion":[],"editorialEvents":[{"content":"https://doi.org/10.1038/s41467-024-53530-9","type":"published","date":"2024-10-30T04:00:00+00:00"}],"editorialNote":"","failedWorkflow":false,"files":[{"id":51791506,"identity":"8294a5c6-5490-4aec-af58-a523e1dd6bc8","added_by":"auto","created_at":"2024-02-29 05:50:18","extension":"jpeg","order_by":1,"title":"Figure 1","display":"","copyAsset":false,"role":"figure","size":413913,"visible":true,"origin":"","legend":"\u003cp\u003e\u003cstrong\u003eDesign concept and principle. \u003c/strong\u003e(\u003cstrong\u003ea\u003c/strong\u003e) Experimental setup and achieved diffraction patterns of the proposed dynamic photomask when the laser beam passes it. (\u003cstrong\u003eb\u003c/strong\u003e) Calculated NLC molecular distributions along the \u003cem\u003ez\u003c/em\u003e-axis driven by an electric field (1 kHz, 400 Vpp), and NLC molecular orientation of \u003cem\u003ex\u003c/em\u003e-\u003cem\u003ez \u003c/em\u003eplane aligning to the electric field lines (E). (\u003cstrong\u003ec\u003c/strong\u003e) Experimentally observed OM image of diffraction pattern, corresponding (\u003cstrong\u003ed\u003c/strong\u003e) 3D surface topography of microstructure obtained via one-step lithography, and (\u003cstrong\u003ee\u003c/strong\u003e) transferred microstructure on silicon wafer at a specific working distance.\u003c/p\u003e","description":"","filename":"floatimage1.jpeg","url":"https://assets-eu.researchsquare.com/files/rs-3992476/v1/a3dd6b70c8961de8c44b83f8.jpeg"},{"id":51791056,"identity":"dbd467ab-1ea9-43fa-8f6a-79b9f33cff48","added_by":"auto","created_at":"2024-02-29 05:42:18","extension":"jpeg","order_by":2,"title":"Figure 2","display":"","copyAsset":false,"role":"figure","size":344945,"visible":true,"origin":"","legend":"\u003cp\u003e\u003cstrong\u003eSpatial evolution of the diffraction patterns. \u003c/strong\u003e(\u003cstrong\u003ea\u003c/strong\u003e) Simulated diffraction patterns (Ⅰ) using an incident wavelength (λ) of 405 nm and experimentally observed OM images at λ of (Ⅱ) 405 nm and (Ⅲ) 532 nm at specific distances (\u003cem\u003ez\u003c/em\u003e), when \u003cem\u003eD\u003c/em\u003e = 20.11, \u003cem\u003eL\u003c/em\u003e = 19.89 μm, and \u003cem\u003eH\u003c/em\u003e = 50 μm. The scale bar denotes 20 μm. (\u003cstrong\u003eb\u003c/strong\u003e) Normalized intensity in the selected yellow dashed line in the OM images of experimental diffraction patterns with \u003cem\u003eD\u003c/em\u003e = 29.87, \u003cem\u003eL\u003c/em\u003e = 10.13 μm\u003cem\u003e \u003c/em\u003eand\u003cem\u003e D\u003c/em\u003e = 35.05, \u003cem\u003eL\u003c/em\u003e = 5.95 μm, when \u003cem\u003eR\u003c/em\u003e = 0.289, \u003cem\u003eH\u003c/em\u003e = 50 μm and λ = 405 nm. (\u003cstrong\u003ec\u003c/strong\u003e) Normalized intensity at a representative dashed line in the simulated diffraction pattern with different LC layer thickness (\u003cem\u003eH\u003c/em\u003e = 1, 5, 9, 30, 50 μm) when \u003cem\u003eD\u003c/em\u003e = 20.11 μm, \u003cem\u003eL\u003c/em\u003e = 19.89 μm, λ = 405 nm and \u003cem\u003eR\u003c/em\u003e = 0.560. (\u003cstrong\u003ed\u003c/strong\u003e) \u003cem\u003eZ\u003c/em\u003e\u003csub\u003eT\u003c/sub\u003e values as a function of the square pitch \u003cem\u003ed\u003c/em\u003e (\u003cem\u003ed = D \u003c/em\u003e+\u003cem\u003e L)\u003c/em\u003e at (Ⅰ) \u003cem\u003eD\u003c/em\u003e = 20.58, \u003cem\u003eL\u003c/em\u003e = 4.42 μm, (Ⅱ) \u003cem\u003eD\u003c/em\u003e = 20.19, \u003cem\u003eL\u003c/em\u003e = 9.81 μm, and (Ⅲ) \u003cem\u003eD\u003c/em\u003e = 29.87, \u003cem\u003eL\u003c/em\u003e = 10.13 μm for circle aperture; (Ⅳ-Ⅸ) \u003cem\u003ed\u003c/em\u003e = 40 μm for octagonal, hexagonal, square, and triangular aperture; (Ⅷ) \u003cem\u003eD\u003c/em\u003e = 30.12, \u003cem\u003eL\u003c/em\u003e = 29.88 μm, and (Ⅸ)\u003cem\u003e D\u003c/em\u003e = 40.23, \u003cem\u003eL\u003c/em\u003e = 39.77 μm for circle aperture when \u003cem\u003eH\u003c/em\u003e = 50 μm, λ = 405 nm. All voltage is 400 Vpp.\u003c/p\u003e","description":"","filename":"floatimage2.jpeg","url":"https://assets-eu.researchsquare.com/files/rs-3992476/v1/476929053929d7b1d2047ad9.jpeg"},{"id":51791060,"identity":"247b85df-d955-4020-9e8b-6856a46e5241","added_by":"auto","created_at":"2024-02-29 05:42:18","extension":"jpeg","order_by":3,"title":"Figure 3","display":"","copyAsset":false,"role":"figure","size":247871,"visible":true,"origin":"","legend":"\u003cp\u003e\u003cstrong\u003eFabrication of multi-height gradients microstructure.\u003c/strong\u003e (\u003cstrong\u003ea\u003c/strong\u003e) Response time and OM images between on and off state at \u003cem\u003ez\u003c/em\u003e = 150 μm. Diffraction patterns of (\u003cstrong\u003eb\u003c/strong\u003e) simulation at \u003cem\u003ez\u003c/em\u003e = 1060 μm and (\u003cstrong\u003ec\u003c/strong\u003e) experiment at \u003cem\u003ez\u003c/em\u003e = 1078 μm, and the corresponding (\u003cstrong\u003ed\u003c/strong\u003e) 2D profile image and (\u003cstrong\u003ee\u003c/strong\u003e) 3D surface topography of the fabricated height gradient microstructures through one-step lithograph. The scale bar denotes 10 μm. (\u003cstrong\u003ef\u003c/strong\u003e) Normalized intensity along the representative dashed line in (c) and (e). The experimental parameters are given as follows: \u003cem\u003eD\u003c/em\u003e = 20.11 μm, \u003cem\u003eL\u003c/em\u003e = 19.89 μm, \u003cem\u003eH\u003c/em\u003e = 50 μm, \u003cem\u003eU\u003c/em\u003e = 400 Vpp, and λ = 405 nm.\u003c/p\u003e","description":"","filename":"floatimage3.jpeg","url":"https://assets-eu.researchsquare.com/files/rs-3992476/v1/4089005e2b16ab71eeb876a6.jpeg"},{"id":51791059,"identity":"af72ac82-dfa8-4328-a2f4-b6df51882b98","added_by":"auto","created_at":"2024-02-29 05:42:18","extension":"jpeg","order_by":4,"title":"Figure 4","display":"","copyAsset":false,"role":"figure","size":313461,"visible":true,"origin":"","legend":"\u003cp\u003e\u003cstrong\u003eFabrication of hierarchicalmicrostructure.\u003c/strong\u003e (\u003cstrong\u003ea\u003c/strong\u003e) Schematic diagram of hierarchical microstructures and holographic image preparation. (\u003cstrong\u003eb\u003c/strong\u003e) Experimentally observed OM images and corresponding to the light intensity of diffraction patterns at \u003cem\u003ez\u003c/em\u003e = 3400 and 4100 μm. (\u003cstrong\u003ec\u003c/strong\u003e) 3D surface topographies of resultant hierarchical microstructures from two exposures. The experimental parameters are given as follows: \u003cem\u003eD\u003c/em\u003e = 20.11 μm, \u003cem\u003eL\u003c/em\u003e = 19.89 μm, \u003cem\u003eH\u003c/em\u003e = 50 μm, \u003cem\u003eU\u003c/em\u003e = 400 Vpp, and λ = 405 nm.\u003c/p\u003e","description":"","filename":"floatimage4.jpeg","url":"https://assets-eu.researchsquare.com/files/rs-3992476/v1/b318debef1864c9401790004.jpeg"},{"id":51791058,"identity":"6aae1047-32f4-4760-ade6-ece24ee47285","added_by":"auto","created_at":"2024-02-29 05:42:18","extension":"jpeg","order_by":5,"title":"Figure 5","display":"","copyAsset":false,"role":"figure","size":301061,"visible":true,"origin":"","legend":"\u003cp\u003e\u003cstrong\u003eOptical and mechanical properties of microstructures.\u003c/strong\u003e (\u003cstrong\u003ea\u003c/strong\u003e) Experimentally observed OM image of diffraction pattern, corresponding (\u003cstrong\u003eb\u003c/strong\u003e) 3D surface topography of microstructures obtained via the lithography: (top) the 3D data model from 3D surface topography and (bottom) the simulated mechanical response of the microstructure at different angles at a specific distance (\u003cem\u003ez\u003c/em\u003e = 3400 μm). (\u003cstrong\u003ec\u003c/strong\u003e) Top view of SEM image of UPs-textured silicon wafer obtained by etching in (B). (\u003cstrong\u003ed\u003c/strong\u003e) Schematic diagram of sunlight reflection on UPs-textured silicon wafer. (\u003cstrong\u003ee\u003c/strong\u003e) Reflectance spectrum of standard silicon wafer, and UPs-textured silicon wafer without and with trapping effects of microstructure responding to sunlight. The experimental parameters are \u003cem\u003eD\u003c/em\u003e = 20.11 μm, \u003cem\u003eL\u003c/em\u003e = 19.89 μm, \u003cem\u003eH\u003c/em\u003e= 50 μm, \u003cem\u003eU\u003c/em\u003e = 400 Vpp, and λ = 405 nm.\u003c/p\u003e","description":"","filename":"floatimage5.jpeg","url":"https://assets-eu.researchsquare.com/files/rs-3992476/v1/e2d9cb813c0ea0288a5ce749.jpeg"},{"id":67918355,"identity":"7a5e9fe8-e489-49ab-82bf-a73d6dad552a","added_by":"auto","created_at":"2024-10-31 07:07:41","extension":"pdf","order_by":0,"title":"","display":"","copyAsset":false,"role":"manuscript-pdf","size":2389415,"visible":true,"origin":"","legend":"","description":"","filename":"manuscript.pdf","url":"https://assets-eu.researchsquare.com/files/rs-3992476/v1/c94c8f72-c8e6-42b4-bb5a-6bb5678dd81d.pdf"},{"id":51791055,"identity":"ac99c667-8784-49f4-891a-b3e277a65d80","added_by":"auto","created_at":"2024-02-29 05:42:18","extension":"pdf","order_by":1,"title":"","display":"","copyAsset":false,"role":"supplement","size":674795,"visible":true,"origin":"","legend":"\u003cp\u003eSupplementary information\u003c/p\u003e","description":"","filename":"Supplementaryinformation.pdf","url":"https://assets-eu.researchsquare.com/files/rs-3992476/v1/25740f0c9339719a0b4391d8.pdf"},{"id":51791062,"identity":"1c464009-cd4b-448e-b1b3-7f1bea2f9664","added_by":"auto","created_at":"2024-02-29 05:42:19","extension":"rar","order_by":2,"title":"","display":"","copyAsset":false,"role":"supplement","size":46330815,"visible":true,"origin":"","legend":"\u003cp\u003eSupplementary Movies\u003c/p\u003e","description":"","filename":"SupplementaryMovies.rar","url":"https://assets-eu.researchsquare.com/files/rs-3992476/v1/5d091731d9991de8eddb9026.rar"}],"financialInterests":"There is \u003cb\u003eNO\u003c/b\u003e Competing Interest.\nThere is no conflict of interest","formattedTitle":"Dynamic photomask directed lithography based on electrically stimulated nematic liquid crystal architectures","fulltext":[{"header":"Introduction","content":"\u003cp\u003eThe emergence of artificial metamaterial has opened new avenues for exploring the unusual electromagnetic, mechanical, optical and theological properties of the materials\u003csup\u003e\u003cspan additionalcitationids=\"CR2 CR3\" citationid=\"CR1\" class=\"CitationRef\"\u003e1\u003c/span\u003e\u0026ndash;\u003cspan citationid=\"CR4\" class=\"CitationRef\"\u003e4\u003c/span\u003e\u003c/sup\u003e. These artificial structures introduce a paradigm for engineering the materials with designable structural properties and thus enabling functions beyond the reach of existing bulky materials. They feature micron/nanoscale characteristics, which facilitates various applications ranging from hierarchical photonic devices\u003csup\u003e\u003cspan citationid=\"CR5\" class=\"CitationRef\"\u003e5\u003c/span\u003e, \u003cspan citationid=\"CR6\" class=\"CitationRef\"\u003e6\u003c/span\u003e\u003c/sup\u003e, electromagnetic and acoustic metamaterials\u003csup\u003e\u003cspan citationid=\"CR7\" class=\"CitationRef\"\u003e7\u003c/span\u003e, \u003cspan citationid=\"CR8\" class=\"CitationRef\"\u003e8\u003c/span\u003e\u003c/sup\u003e, mechanical metamaterials\u003csup\u003e\u003cspan citationid=\"CR9\" class=\"CitationRef\"\u003e9\u003c/span\u003e, \u003cspan citationid=\"CR10\" class=\"CitationRef\"\u003e10\u003c/span\u003e\u003c/sup\u003e, and thermal energy transfer\u003csup\u003e\u003cspan citationid=\"CR11\" class=\"CitationRef\"\u003e11\u003c/span\u003e\u003c/sup\u003e.\u003c/p\u003e \u003cp\u003eSo far, artificial structures have been primarily fabricated using lithography techniques, including two-photon lithography (TPL)\u003csup\u003e\u003cspan citationid=\"CR12\" class=\"CitationRef\"\u003e12\u003c/span\u003e\u003c/sup\u003e, electron beam lithography (EBL)\u003csup\u003e\u003cspan citationid=\"CR13\" class=\"CitationRef\"\u003e13\u003c/span\u003e\u003c/sup\u003e, nanoimprint lithography (NIL)\u003csup\u003e\u003cspan citationid=\"CR14\" class=\"CitationRef\"\u003e14\u003c/span\u003e\u003c/sup\u003e, capillary force lithography (CFL)\u003csup\u003e\u003cspan citationid=\"CR15\" class=\"CitationRef\"\u003e15\u003c/span\u003e\u003c/sup\u003e, and traditional three-dimensional (3D) printing\u003csup\u003e\u003cspan citationid=\"CR16\" class=\"CitationRef\"\u003e16\u003c/span\u003e\u003c/sup\u003e. Generally, TPL has the capability of producing high-resolution structures with feature size down to 200 nm\u003csup\u003e\u003cspan citationid=\"CR17\" class=\"CitationRef\"\u003e17\u003c/span\u003e, \u003cspan citationid=\"CR18\" class=\"CitationRef\"\u003e18\u003c/span\u003e\u003c/sup\u003e. However, similar to the EBL relying on pixel-by-pixel writing process\u003csup\u003e\u003cspan citationid=\"CR19\" class=\"CitationRef\"\u003e19\u003c/span\u003e\u003c/sup\u003e, the limited-throughput caused by seriality renders TPL time-consuming to pattern large-area microstructures\u003csup\u003e\u003cspan citationid=\"CR17\" class=\"CitationRef\"\u003e17\u003c/span\u003e, \u003cspan citationid=\"CR18\" class=\"CitationRef\"\u003e18\u003c/span\u003e\u003c/sup\u003e. Although this challenge can be partially mitigated by the high-throughput NIL and CFL which are particularly suitable for large-area patterning, they either heavily rely on the master imprint mold or lack flexibility in geometric design\u003csup\u003e\u003cspan citationid=\"CR14\" class=\"CitationRef\"\u003e14\u003c/span\u003e, \u003cspan citationid=\"CR20\" class=\"CitationRef\"\u003e20\u003c/span\u003e, \u003cspan citationid=\"CR21\" class=\"CitationRef\"\u003e21\u003c/span\u003e\u003c/sup\u003e. Alternatively, traditional 3D printing technique can offer great design flexibility, but it suffers from bottlenecks in patterning accuracy and inherent limitations in materials\u003csup\u003e\u003cspan citationid=\"CR22\" class=\"CitationRef\"\u003e22\u003c/span\u003e\u003c/sup\u003e. Generally, aforementioned lithography techniques either lean on static masks or have relatively low fabrication accuracy. In principle, the preparation of conventional artificial structures with single height gradient is relatively straightforward, whereas multi-height gradients should turn to top-down or bottom-up methods\u003csup\u003e\u003cspan additionalcitationids=\"CR24 CR25\" citationid=\"CR23\" class=\"CitationRef\"\u003e23\u003c/span\u003e\u0026ndash;\u003cspan citationid=\"CR26\" class=\"CitationRef\"\u003e26\u003c/span\u003e\u003c/sup\u003e. Hence, the cost-effective preparation method of hierarchical structures with micron/nanoscale features remains challenging.\u003c/p\u003e \u003cp\u003eTraditionally, the fabrication of hierarchical structures based on static masks adopts multiple lithography processes requiring the successive replacement of different masks, which is sophisticated and challenging due to the difficulties in accurately aligning the patterns on the masks\u003csup\u003e\u003cspan citationid=\"CR13\" class=\"CitationRef\"\u003e13\u003c/span\u003e, \u003cspan additionalcitationids=\"CR28\" citationid=\"CR27\" class=\"CitationRef\"\u003e27\u003c/span\u003e\u0026ndash;\u003cspan citationid=\"CR29\" class=\"CitationRef\"\u003e29\u003c/span\u003e\u003c/sup\u003e. Although this challenge can be alleviated by employing multiplexed lithography, allowing for production of various multilevel microstructures, the fabrication of the mask remains complicated\u003csup\u003e\u003cspan citationid=\"CR30\" class=\"CitationRef\"\u003e30\u003c/span\u003e\u003c/sup\u003e. Recently, there has been an increasing attention on the temporal and spatial evolution facilitated by electrically stimulated liquid crystal (LC), as highlighted in these studies\u003csup\u003e\u003cspan citationid=\"CR31\" class=\"CitationRef\"\u003e31\u003c/span\u003e, \u003cspan citationid=\"CR32\" class=\"CitationRef\"\u003e32\u003c/span\u003e\u003c/sup\u003e. Nematic LC (NLC) stands out as a simple and versatile soft material characterized by optical birefringence and ability to assemble into multifarious architectures under the geometric confinement and external stimuli, thus generating dynamic diffraction patterns with designable properties\u003csup\u003e\u003cspan additionalcitationids=\"CR34 CR35 CR36 CR37\" citationid=\"CR33\" class=\"CitationRef\"\u003e33\u003c/span\u003e\u0026ndash;\u003cspan citationid=\"CR38\" class=\"CitationRef\"\u003e38\u003c/span\u003e\u003c/sup\u003e. Hence, these dynamic patterns are highly promising in photolithography as metamask for preparing structures with micron/nanoscale features onto the photosensitive materials through one-step lithography.\u003c/p\u003e \u003cp\u003eHerein, we report a dynamic photomask for directed lithography, which is driven by diffraction pattern from assembling the electrically stimulated NLC molecules into multifarious architectures. The virtual metamasks are composed of reconfigurable and switchable diffraction patterns of the NLC architectures, which are enriched with information of grayscale and can be used as bridge in lithography. We adopt the Landau-de Gennes\u0026rsquo;s Q tensor and nonuniform finite difference method to theoretically predict the optical behavior of the NLC architectures under external stimuli. The resultant diffraction pattern, functioning as the metamask, successfully fabricates two-height gradients microstructure on negative photoresist (HN-018) using one-step lithography process, and the obtained microstructure has feature size about 3.2 times smaller than the initial electrode pattern. This also can produce hierarchical microstructure through in-situ manipulation of the working distance and simultaneous exposures. Moreover, the microstructure is transferred onto a silicon wafer through wet etching, yielding structures endowed with distinctive optical and mechanical properties that align with the diffraction pattern. Remarkably, our metamask is independent from incident wavelengths, making it compatible with a broad range of materials for lithography. This approach streamlines the controlled and flexible production of various microstructures, distinguishing itself through its simplicity, cost-effectiveness, and efficiency in manufacturing. The resulting multi-functional microstructures are highly advantageous for a multitude of applications.\u003c/p\u003e"},{"header":"Results","content":"\u003cdiv id=\"Sec3\" class=\"Section2\"\u003e\n\u003ch2\u003ePrinciple of lithography utilizing metamask\u003c/h2\u003e\n\u003cp\u003eFigure \u003cspan class=\"InternalRef\"\u003e1\u003c/span\u003e depicts the basic principle of the proposed dynamic photomask directed lithography. \u003cstrong\u003eFigure. 1a\u003c/strong\u003e and \u003cstrong\u003eSupplementary Fig.\u0026nbsp;1\u003c/strong\u003e show the schematic setup to create the metamask based on the electrically stimulated assembly NLC molecules into architectures. The continuous-wave laser beam with working wavelength of 405 nm is expanded and then collimated by the lenses and aperture. The collimated beam is converted to circularly polarized light and then modulated by the NLC sample, generating coherent diffraction patterns that spatially evolve along the propagation direction (Fig.\u0026nbsp;\u003cspan class=\"InternalRef\"\u003e1\u003c/span\u003ea). The sample of the dynamic NLC photomask is consisted of uniaxial LC material (5CB, with positive dielectric anisotropy) sandwiched between a top substrate coated with uniform ITO and a bottom substrate with patterned ITO coated with a passivation layer (Hyflon) (\u003cstrong\u003eSupplementary Fig.\u0026nbsp;1\u003c/strong\u003e). In principle, the optical axis of 5CB molecules undergoes constant fluctuations attributed to thermal movements, and hence only a small amount of energy is sufficient to reorient their directors. This remarkable characteristic allows for manipulating the NLC molecules with an external electric field. We calculate the molecular distributions (LC thickness: 50 \u0026micro;m) along the \u003cem\u003ez\u003c/em\u003e-axis and \u003cem\u003ex\u003c/em\u003e-\u003cem\u003ez\u003c/em\u003e plane in response to the applied electric field (1 kHz, 400 Vpp) (Fig.\u0026nbsp;\u003cspan class=\"InternalRef\"\u003e1\u003c/span\u003eb and \u003cstrong\u003eSupplementary Fig.\u0026nbsp;2\u003c/strong\u003e). The NLC molecular directors tend to exhibit uniform state (90\u0026deg;) within the conductive ITO region, due to the uniform electric field distribution across the LC layer in the vertical direction (Fig.\u0026nbsp;\u003cspan class=\"InternalRef\"\u003e1\u003c/span\u003eb). On the contrary, in the circular aperture region without ITO, the NLC molecular directors with tilt angles varying from 33.23 to 90\u0026deg; are circularly symmetric in the transverse planes along \u003cem\u003ez\u003c/em\u003e-axis, and follow the electric field in \u003cem\u003ex-z\u003c/em\u003e plane, leading to a controllable phase profile. Consequently, when the laser beam passes through this region with specific phase retardation, typical diffraction patterns are generated (Fig.\u0026nbsp;\u003cspan class=\"InternalRef\"\u003e1\u003c/span\u003ea). Large quantity of complex diffraction patterns resulted from the constructive or destructive interference between neighboring patterns, appear in the propagation direction, thus providing a promising platform for photomask. The intensity distribution of one of the diffraction patterns is illustrated by the optical microscope (OM) image (Fig.\u0026nbsp;\u003cspan class=\"InternalRef\"\u003e1\u003c/span\u003ec). When it is employed as metamask to pattern photosensitive materials (negative photoresist HN-018), microstructure with 3D surface topography is obtained after one-step standard photolithographic process \u003cstrong\u003e(\u003c/strong\u003eFig.\u0026nbsp;\u003cspan class=\"InternalRef\"\u003e1\u003c/span\u003ed). Alternatively, we can also realize a new microstructure (Fig.\u0026nbsp;\u003cspan class=\"InternalRef\"\u003e1\u003c/span\u003ee) after transferring the pattern in Fig.\u0026nbsp;\u003cspan class=\"InternalRef\"\u003e1\u003c/span\u003ed to a silicon wafer by wet etching, providing a promising technique for microelectromechanical systems (MEMS).\u003c/p\u003e\n\u003c/div\u003e\n\u003cdiv id=\"Sec4\" class=\"Section2\"\u003e\n\u003ch2\u003eModulation of diffraction patterns\u003c/h2\u003e\n\u003cp\u003eWe firstly simulate the optical performance of the NLC architectures under the stimulation of electric field after efficiently calculating the molecular director configuration in Fig.\u0026nbsp;\u003cspan class=\"InternalRef\"\u003e1\u003c/span\u003eb. Here, typical parameters of a circle electrode pattern are given as follows: diameter of the electrode (\u003cem\u003eD\u003c/em\u003e\u0026thinsp;=\u0026thinsp;20.11 \u0026micro;m), spacing between neighboring electrode patterns (\u003cem\u003eL\u003c/em\u003e\u0026thinsp;=\u0026thinsp;19.89 \u0026micro;m), and thickness of LC layer (\u003cem\u003eH\u003c/em\u003e\u0026thinsp;=\u0026thinsp;50 \u0026micro;m). The working wavelength of the incident continuous-wave laser beam is 405 nm. The driving alternating voltage (AC) of square wave is set at a frequency of 1 kHz and 400 peak-to-peak value (Vpp)\u003csup\u003e\u003cspan class=\"CitationRef\"\u003e39\u003c/span\u003e, \u003cspan class=\"CitationRef\"\u003e40\u003c/span\u003e\u003c/sup\u003e. Figure\u0026nbsp;\u003cspan class=\"InternalRef\"\u003e2\u003c/span\u003ea \u003cstrong\u003e(Ⅰ)\u003c/strong\u003e shows the simulated images of diffraction patterns propagating along the \u003cem\u003ez\u003c/em\u003e-axis at specific distance: \u003cem\u003ez\u003c/em\u003e\u0026thinsp;=\u0026thinsp;0, 335.0, 1401.0, 3188.0, and 4176.0 \u0026micro;m. The diffraction pattern on the LC layer surface is determined to be \u003cem\u003ez\u003c/em\u003e\u0026thinsp;=\u0026thinsp;0 \u0026micro;m, taking the shape of circle. As \u003cem\u003ez\u003c/em\u003e increases, diverse diffraction patterns with different complexity appear within the circular aperture, morphing from flower-like shapes at \u003cem\u003ez\u003c/em\u003e\u0026thinsp;=\u0026thinsp;335.0 \u0026micro;m to squares and ultimately backed to circles in a cyclic manner. Correspondingly, we experimentally record the OM images of diffraction patterns at \u003cem\u003ez\u003c/em\u003e\u0026thinsp;=\u0026thinsp;85.3, 419.9, 1485.0, 3250.0, and 4194.9 \u0026micro;m, which are consistent with the simulation results (Fig.\u0026nbsp;\u003cspan class=\"InternalRef\"\u003e2\u003c/span\u003ea \u003cstrong\u003e(Ⅱ)\u003c/strong\u003e). We also provide two movies to illustrate the dynamic evolution of diffraction patterns in the simulation and experiment (\u003cstrong\u003eSupplementary Movies 1 and 2\u003c/strong\u003e). These movies show that the diffraction patterns repeat themselves along the propagation direction after a regular distance away from the exit plane, following the theory of Talbot effect\u003csup\u003e\u003cspan class=\"CitationRef\"\u003e41\u003c/span\u003e\u003c/sup\u003e. This regular distance is widely known as Talbot length and given by \u003cspan class=\"InlineEquation\"\u003e\u003cspan class=\"mathinline\"\u003e\\(Z=2\\left( {{{{d^2}} \\mathord{\\left/ {\\vphantom {{{d^2}} \\lambda }} \\right. \\kern-0pt} \\lambda }} \\right)\\)\u003c/span\u003e\u003c/span\u003e, where \u003cem\u003ed\u003c/em\u003e is a pitch (\u003cspan class=\"InlineEquation\"\u003e\u003cspan class=\"mathinline\"\u003e\\(d=D+L\\)\u003c/span\u003e\u003c/span\u003e) and \u0026lambda; is the incident wavelength. Since the image at \u003cspan class=\"InlineEquation\"\u003e\u003cspan class=\"mathinline\"\u003e\\({{{d^2}} \\mathord{\\left/ {\\vphantom {{{d^2}} \\lambda }} \\right. \\kern-0pt} \\lambda }\\)\u003c/span\u003e\u003c/span\u003e corresponds to a negative image, thus we can simply consider half of the Talbot length as the periodic length (\u003cspan class=\"InlineEquation\"\u003e\u003cspan class=\"mathinline\"\u003e\\({Z_{\\text{T}}}={{{d^2}} \\mathord{\\left/ {\\vphantom {{{d^2}} \\lambda }} \\right. \\kern-0pt} \\lambda }\\)\u003c/span\u003e\u003c/span\u003e) to avoid the repetition of optical patterns. The simulated and experimental \u003cspan class=\"InlineEquation\"\u003e\u003cspan class=\"mathinline\"\u003e\\({Z_{\\text{T}}}\\)\u003c/span\u003e\u003c/span\u003e values are estimated to be 4176.0 and 4194.9 \u0026micro;m, indicating a good match, whereas the theoretical \u003cspan class=\"InlineEquation\"\u003e\u003cspan class=\"mathinline\"\u003e\\({Z_{\\text{T}}}\\)\u003c/span\u003e\u003c/span\u003e value is 3950.6 \u0026micro;m based on the assumptions of working wavelength of 405 nm and a pitch of 40 \u0026micro;m. This minor difference between the simulated and theoretical values can be attributed to the lack of consideration for the cell thickness in the calculation. The simulated \u003cspan class=\"InlineEquation\"\u003e\u003cspan class=\"mathinline\"\u003e\\({Z_{\\text{T}}}\\)\u003c/span\u003e\u003c/span\u003e value includes the propagation distance between the LC layer and the glass and air. Moreover, it can be observed that \u003cspan class=\"InlineEquation\"\u003e\u003cspan class=\"mathinline\"\u003e\\({Z_{\\text{T}}}\\)\u003c/span\u003e\u003c/span\u003e is inversely proportional to the wavelength, implying that the dynamic change of diffraction pattern can be tuned with the wavelength. When the wavelength is 532 nm, \u003cspan class=\"InlineEquation\"\u003e\u003cspan class=\"mathinline\"\u003e\\({Z_{\\text{T}}}\\)\u003c/span\u003e\u003c/span\u003e value is shortened by 0.76 times (Fig.\u0026nbsp;\u003cspan class=\"InternalRef\"\u003e2\u003c/span\u003ea \u003cstrong\u003e(III)\u003c/strong\u003e). However, the same diffraction patterns can be obtained at \u003cem\u003ez\u003c/em\u003e\u0026thinsp;=\u0026thinsp;0.9, 319.0, 1111.0, 2470.0, and 3210.0 \u0026micro;m. This helps to demonstrate that the sample is broadband, which is a significant advantage of the NLC photomask for lithography, due to the greatly expanding selection range of photosensitive materials. To compare the patterns under different conditions, a dimensionless ratio \u003cem\u003eR\u003c/em\u003e applicable throughout the entire study is defined as \u003cspan class=\"InlineEquation\"\u003e\u003cspan class=\"mathinline\"\u003e\\({Z \\mathord{\\left/ {\\vphantom {Z {{Z_{\\text{T}}}}}} \\right. \\kern-0pt} {{Z_{\\text{T}}}}}\\)\u003c/span\u003e\u003c/span\u003e.\u003c/p\u003e\n\u003cp\u003eThe pluralistic morphology of the diffraction pattern can also be modulated by changing the electrode shapes (\u003cstrong\u003eSupplementary Fig.\u0026nbsp;3\u003c/strong\u003e). Moreover, it is very reasonable to infer that the diffraction pattern can also be tuned by the electrode parameters. This is demonstrated by the experiments in \u003cstrong\u003eSupplementary Fig.\u0026nbsp;4a\u003c/strong\u003e, where two samples (\u003cem\u003eD\u003c/em\u003e\u0026thinsp;=\u0026thinsp;29.87, \u003cem\u003eL\u003c/em\u003e\u0026thinsp;=\u0026thinsp;10.13 \u0026micro;m and \u003cem\u003eD\u003c/em\u003e\u0026thinsp;=\u0026thinsp;35.05, \u003cem\u003eL\u003c/em\u003e\u0026thinsp;=\u0026thinsp;5.95 \u0026micro;m) with the same pitch but different \u003cem\u003eL\u003c/em\u003e and \u003cem\u003eD\u003c/em\u003e are fabricated and optically characterized. In order to better illustrate the properties of diffraction pattern, we plot the normalized intensity of gray value on a representative line. The intensity in the selected yellow dashed line in the OM images reveals that the diffraction patterns contain four gray levels, four peaks and valleys when \u003cem\u003eD\u003c/em\u003e\u0026thinsp;=\u0026thinsp;29.87 and \u003cem\u003eL\u003c/em\u003e\u0026thinsp;=\u0026thinsp;10.13 \u0026micro;m (Fig.\u0026nbsp;\u003cspan class=\"InternalRef\"\u003e2\u003c/span\u003eb). The gray levels represent the gradients, and the peak or valley along the \u003cem\u003ex\u003c/em\u003e-axis reflects an indicator of microstructure. However, the features increase to five and six when \u003cem\u003eD\u003c/em\u003e\u0026thinsp;=\u0026thinsp;35.05 and \u003cem\u003eL\u003c/em\u003e\u0026thinsp;=\u0026thinsp;5.95 \u0026micro;m. This is because the small deflection angle (28.20\u0026deg;) of the electrically stimulated NLC molecules can lead to maximum refraction of light (\u003cstrong\u003eSupplementary Fig.\u0026nbsp;4b\u003c/strong\u003e), resulting in an increase of interference intensity between the neighboring the electrode patterns when \u003cem\u003eD\u003c/em\u003e\u0026thinsp;=\u0026thinsp;35.05 and \u003cem\u003eL\u003c/em\u003e\u0026thinsp;=\u0026thinsp;4.95 \u0026micro;m. Compared to the case of \u003cem\u003eD\u003c/em\u003e\u0026thinsp;=\u0026thinsp;29.87 and \u003cem\u003eL\u003c/em\u003e\u0026thinsp;=\u0026thinsp;10.13 \u0026micro;m with a minimum angle of 30.49\u0026deg;, the thickness of the electrically stimulated NLC molecules is also increasing, which plays a synergistic role in the complexity of diffraction patterns (\u003cstrong\u003eSupplementary Fig.\u0026nbsp;4b\u003c/strong\u003e). Therefore, it is also imperative to delve into exploring how LC layer thickness affects the gray levels of diffraction patterns when the \u003cem\u003eD\u003c/em\u003e and \u003cem\u003eL\u003c/em\u003e remain unchanged. As aforementioned in Fig.\u0026nbsp;\u003cspan class=\"InternalRef\"\u003e1\u003c/span\u003eb, the orientations of the NLC molecules experience sufficiently perturbations when the LC thickness falls below 9 \u0026micro;m when \u003cem\u003eD\u003c/em\u003e\u0026thinsp;=\u0026thinsp;20.11 and \u003cem\u003eL\u003c/em\u003e\u0026thinsp;=\u0026thinsp;19.89 \u0026micro;m. The normalized intensity (Fig.\u0026nbsp;\u003cspan class=\"InternalRef\"\u003e2\u003c/span\u003ec) along the designated black dashed line in the simulated diffraction pattern (\u003cstrong\u003eSupplementary Fig.\u0026nbsp;5a\u003c/strong\u003e), showcases discernible variations corresponding to different LC layer thickness (\u003cem\u003eH\u003c/em\u003e\u0026thinsp;=\u0026thinsp;1, 5, 9, 30, 50 \u0026micro;m). At a thickness of 1 \u0026micro;m, the intensity remains a fixed value out nuanced gradients of gray levels. However, three distinct gray levels emerge with a relatively low contrast at a LC thickness of 5 \u0026micro;m. When the LC thickness is beyond 9 \u0026micro;m, the diffraction pattern characterized by pronounced contrast remains virtually unaltered. This phenomenon can be attributed to the vertical alignment of NLC molecules near the upper electrode, and thus there is an absence of birefringence, leading to negligible impact on the diffraction pattern. Moreover, owing to the small extinction coefficient of 5CB\u003csup\u003e\u003cspan class=\"CitationRef\"\u003e42\u003c/span\u003e\u003c/sup\u003e, the transmitted light intensity exhibits remarkable stability even the LC thickness reaching 50 \u0026micro;m. Simultaneously, these experimentally captured diffraction patterns adopt consistently aligned when \u003cem\u003eH\u003c/em\u003e\u0026thinsp;=\u0026thinsp;30, 50, 80, and 100 \u0026micro;m (\u003cstrong\u003eSupplementary Fig.\u0026nbsp;5b\u003c/strong\u003e). Moreover, we also investigate the other electrode parameter and find that the diffraction patterns are highly adjustable (\u003cstrong\u003eSupplementary Fig.\u0026nbsp;6\u003c/strong\u003e).\u003c/p\u003e\n\u003cp\u003eAlthough these diffraction patterns are reconfigurable, they are periodic and follow the Talbot length. Figure\u0026nbsp;\u003cspan class=\"InternalRef\"\u003e2\u003c/span\u003ed shows the corresponding \u003cspan class=\"InlineEquation\"\u003e\u003cspan class=\"mathinline\"\u003e\\({Z_{\\text{T}}}\\)\u003c/span\u003e\u003c/span\u003e values as a function of the square pitch \u003cem\u003ed\u003c/em\u003e. A linear correlation of \u003cspan class=\"InlineEquation\"\u003e\u003cspan class=\"mathinline\"\u003e\\({Z_{\\text{T}}}=2.47{d^2}+190.79\\)\u003c/span\u003e\u003c/span\u003e (\u003cem\u003eR\u003c/em\u003e\u003csup\u003e2\u003c/sup\u003e\u0026thinsp;=\u0026thinsp;0.99) can be observed in the range of 25\u0026thinsp;\u0026minus;\u0026thinsp;80 \u0026micro;m. Similarly, the \u003cspan class=\"InlineEquation\"\u003e\u003cspan class=\"mathinline\"\u003e\\({Z_{\\text{T}}}\\)\u003c/span\u003e\u003c/span\u003e values match excellently with the same pitch of 40 \u0026micro;m when the electrode shapes are circular, octagonal, hexagonal, square, and triangular apertures in the red dashed line of Fig.\u0026nbsp;\u003cspan class=\"InternalRef\"\u003e2\u003c/span\u003ec. \u003cstrong\u003eSupplementary Fig.\u0026nbsp;5c\u003c/strong\u003e also shows the \u003cspan class=\"InlineEquation\"\u003e\u003cspan class=\"mathinline\"\u003e\\({Z_{\\text{T}}}\\)\u003c/span\u003e\u003c/span\u003e values remain nearly constant at different LC layer thickness, with the slight discrepancies attributed to the variations in LC layer thickness. The cyclic periodicity of the diffraction pattern in the direction of light propagation allows for greatly selecting metamask for lithography.\u003c/p\u003e\n\u003c/div\u003e\n\u003cdiv id=\"Sec5\" class=\"Section2\"\u003e\n\u003ch2\u003eFabrication of microstructure\u003c/h2\u003e\n\u003cp\u003eThe efficiency of lithography and stability of photomask are two crucial factors in practical application. In this study, the applied electric field requires certain relaxation time to trigger the rotation of NLC molecules towards the state of minimum total free energy. The measured native response on-time is 477 ms following the case with 400 Vpp (Fig.\u0026nbsp;\u003cspan class=\"InternalRef\"\u003e3\u003c/span\u003ea). Subsequently, upon deactivating the electric field, the NLC molecules revert to their original state within a timeframe of 480 ms. This response time is at least four orders of magnitude smaller than the entire lithography process, proving that our proposal is efficient enough for lithography. Furthermore, the OM images in Fig.\u0026nbsp;\u003cspan class=\"InternalRef\"\u003e3\u003c/span\u003ea affirm that the transitions between stable configurations are entirely reversible, maintaining ultrahigh stability even after 100 switching cycles. Hence, the assembled NLC architectures, functioning as a photomask generator, have the advantages of fast response, excellent stability, and outstanding repeatability, rendering them exceptionally well-suited for the fabrication of microstructure for active applications.\u003c/p\u003e\n\u003cp\u003eIn our strategy, the diffraction patterns formed by NLC architectures contain gray information, which can serve as gray mask to pattern the multi-height gradient microstructure. Although microstructures featuring multi-height gradients have been widely utilized in fields such as optics and surface engineering\u003csup\u003e\u003cspan class=\"CitationRef\"\u003e3\u003c/span\u003e, \u003cspan class=\"CitationRef\"\u003e43\u003c/span\u003e\u003c/sup\u003e, efficient fabrication remains a challenge. Here, we prove the feasibility of using this gray mask to prepare a typical multi-height gradient microstructure through one-step lithography. We choose the diffraction pattern of sample with circular electrode array (\u003cem\u003ed\u003c/em\u003e\u0026thinsp;=\u0026thinsp;40 \u0026micro;m, \u003cem\u003eH\u003c/em\u003e\u0026thinsp;=\u0026thinsp;50 \u0026micro;m) at position of 1060 \u0026micro;m (Fig.\u0026nbsp;\u003cspan class=\"InternalRef\"\u003e3\u003c/span\u003eb). The normalized intensity of the dashed line in the simulated diffraction pattern exhibits a minimum 6 gray levels (\u003cstrong\u003eSupplementary Fig.\u0026nbsp;7\u003c/strong\u003e). Each peak or valley along the \u003cem\u003ex\u003c/em\u003e-axis reflects an indicator of lithographic resolution, with simulation results suggesting an achievable resolution of 1.2 \u0026micro;m. After using this diffraction pattern (Fig.\u0026nbsp;\u003cspan class=\"InternalRef\"\u003e3\u003c/span\u003ec) as a metamask for lithography, the diffraction pattern is successfully replicated onto the negative HN-018 photoresist coated on the glass by one-step lithography, which can be partially demonstrated by the 2D profile image of microstructure (Fig.\u0026nbsp;\u003cspan class=\"InternalRef\"\u003e3\u003c/span\u003ed). The resulting 3D surface topography image displays at least two-height gradients on photosensitive materials with an 8 \u0026micro;m thickness (Fig.\u0026nbsp;\u003cspan class=\"InternalRef\"\u003e3\u003c/span\u003ee). The 1st gradient microstructure corresponds to the glass substrate, as evidenced by the region with null diffraction light. The average size measures 6.2 \u0026micro;m, which is 3.2 times smaller than the designed electrode size, as shown in the red dotted box in Fig.\u0026nbsp;\u003cspan class=\"InternalRef\"\u003e3\u003c/span\u003ee. The 2nd gradient microstructure displays a thickness ranging between 4 and 6 \u0026micro;m, while the 3rd gradient manifests a thickness of approximately 8 \u0026micro;m, aligning with the initial thickness of the photoresist layer. Figure\u0026nbsp;\u003cspan class=\"InternalRef\"\u003e3\u003c/span\u003ef plots the normalized intensity and height of the selected dashed line containing 3 levels on the image of Figs.\u0026nbsp;\u003cspan class=\"InternalRef\"\u003e3\u003c/span\u003ec,e. The 2nd level has subtle difference within a range, attributing to the low accuracy of laser. This approach for fabricating multi-height gradient microstructures through one-step lithography is time-saving and cost-effective.\u003c/p\u003e\n\u003cp\u003eOwing to the high freedom of this photomask, hierarchical microstructures could also be easily generated in-situ using the one-step multilayer photolithography technique. Specifically, the sample undergoes exposure to the first target light field and then to the second light field at another longitudinal location, both originating from the same photomask (Fig.\u0026nbsp;\u003cspan class=\"InternalRef\"\u003e4\u003c/span\u003ea). Through this process, the two light fields are superimposed and embedded together into the same sample, hence the hierarchical microstructure can be realized through rather simple lithography process. Theoretically, holographic image through incorporation of multiple into the same hierarchical 3D microstructure can be achieved by multi-exposing process (Fig.\u0026nbsp;\u003cspan class=\"InternalRef\"\u003e4\u003c/span\u003ea). As a proof of concept, we experimentally fabricate a hierarchical microstructure by superimposing two metamask, namely two diffraction patterns (Fig.\u0026nbsp;\u003cspan class=\"InternalRef\"\u003e4\u003c/span\u003eb). The sample of HN-018 photoresist coated on glass is initially exposed at \u003cem\u003ez\u003c/em\u003e\u0026thinsp;=\u0026thinsp;3400 \u0026micro;m and then mechanically moved to 4100 \u0026micro;m for second exposure. Ultimately, three levels microstructure is achieved after developing. The 3D surface topography image of resultant hierarchical microstructure shows that the 1st level microstructure corresponds to the glass substrate, the 2nd level microstructure is formed by the first exposure, and the 3rd level microstructure emerges from the combining effects of the two exposures, resulting in the highest gradients (Fig.\u0026nbsp;\u003cspan class=\"InternalRef\"\u003e4\u003c/span\u003ec). It should be emphasized that the dynamic photomask for lithography facilitates the creation of hierarchical microstructures in a novel manner, avoiding alignment errors that may arise in multiple lithography compared to EBL\u003csup\u003e\u003cspan class=\"CitationRef\"\u003e13\u003c/span\u003e\u003c/sup\u003e.\u003c/p\u003e\n\u003cp\u003eNaturally, the realization of single-layer microstructure on the photosensitive material (HN-018) photoresist coated on the silicon wafer is possible through using our metamask (Fig.\u0026nbsp;\u003cspan class=\"InternalRef\"\u003e5\u003c/span\u003ea). The recorded 3D surface topography image after lithography aligns closely with the OM image (Fig.\u0026nbsp;\u003cspan class=\"InternalRef\"\u003e5\u003c/span\u003eb). Subsequently, leveraging the derived 3D surface topography of microstructure, the mechanical performance of the obtained material is calculated under the 5\u0026times;10\u003csup\u003e8\u003c/sup\u003e N/m\u003csup\u003e2\u003c/sup\u003e stress using the open-source COMSOL software (Fig.\u0026nbsp;\u003cspan class=\"InternalRef\"\u003e5\u003c/span\u003eb). It is found that the microstructure is anisotropic and possesses a period of 180\u0026deg;. Such kind of anisotropic microstructural materials plays a key role in areas such as the human brain or tendons\u003csup\u003e\u003cspan class=\"CitationRef\"\u003e10\u003c/span\u003e\u003c/sup\u003e. Apart from the demonstration of producing anisotropic microstructure, we transfer the resultant microstructures from the photosensitive material to the silicon wafer by a wet etching process (12.5 wt% TMAH, 300 rpm, 80 ℃, 5 min). The scanning electron microscopy (SEM) image of the produced microstructure (Fig.\u0026nbsp;\u003cspan class=\"InternalRef\"\u003e5\u003c/span\u003ec) illustrates that there is bowl-like structure from a similar square master microstructure, characterized by numerous random upright pyramids (UPs) on the surface. In contrast, the numbers of UPs on the surface decrease in case without microstructure under the same experiment condition (\u003cstrong\u003eSupplementary Fig.\u0026nbsp;8\u003c/strong\u003e). It has been already proved that these textured surfaces which are covered by UPs are promising for manufacturing high-efficiency silicon solar cells\u003csup\u003e\u003cspan class=\"CitationRef\"\u003e44\u003c/span\u003e, \u003cspan class=\"CitationRef\"\u003e45\u003c/span\u003e\u003c/sup\u003e. As depicted in Figs.\u0026nbsp;\u003cspan class=\"InternalRef\"\u003e5\u003c/span\u003ed,e, the reflectance spectrum shows that when the standard silicon wafer as a baseline is thought 100%, the overall average reflectance of the textured surfaces covered with UPs but that without trapping of microstructure is 60%. In contrast, the overall average reflectance can reduce 19%, because the trapping effects of microstructure can be generally understood by the multiple reflection that maximizes the absorption of the incident light. It implies that the microstructures can be transferred onto the silicon wafer, holding the promising in the high-efficiency solar energy harvesting.\u003c/p\u003e\n\u003c/div\u003e"},{"header":"Discussion","content":"\u003cp\u003eWe have developed a cost-saving methodology of harnessing electrically driven NLC assembly architectures to craft a dynamic photomask. Our study demonstrates that modulating the spatially localized orientations of the NLC molecules enables the tuning of the wavefront of the incident laser beam, and consequently leads to intricate diffraction patterns. These diffraction patterns are enriched with grayscale information, which may function as metamask and serve as powerful catalysts for lithography. We successfully prepare the multi-height gradients microstructure onto photosensitive materials (HN-018) by using our proposed metamask. Furthermore, based on the high freedom of the photomask in the propagation direction owing to the coherence between neighborhood electrode patterns, we achieve a kind of hierarchical microstructures through in-situ modulation of work distance from sample photomask. In comparison with the traditional multilayered photolithography methods for fabricating hierarchical microstructures, our proposal eliminates intermediate alignment steps and significantly enhances the efficiency. Remarkably, the microstructure can be transferred onto silicon wafer, and the ensuing microstructures featuring random upright pyramid shapes showcase good optical performance, expanding the application of this methodology. However, we notice in the experiment that the resolution and height gradient of the obtained microstructures deviated from perfection in comparison to the simulation. Envision an enhancement in our work, enhancing the uniformity and power output of the laser, reducing the pattern size, or using high-power ultraviolet laser will lead to better precision, more height gradients and even nanoscale structures. Furthermore, the established simulation method serves as a valuable predictive tool, successfully forecasting a spectrum of diffraction patterns. Looking forward, our vision encompasses the capability to create arbitrary multilevel structures even holographic image through the pre-superimposition of meticulously designed patterns. These strides open expansive application possibilities for customizable metamaterials across various fields such as mechanics, optics, photonics, electricity and so on.\u003c/p\u003e"},{"header":"Materials and methods","content":"\u003cdiv id=\"Sec8\" class=\"Section2\"\u003e \u003ch2\u003eExperimental design of photomask\u003c/h2\u003e \u003cp\u003eWe fabricated the electrode arrays using a standard lithography process. Initially, the ITO substrate was cleaned with a 4 wt% alkaline solution, followed by rinsing with DI water and drying with nitrogen blowing. A positive-type photoresist (SUN-120P) was spin-coated (step 1: 500 rpm for 5 s; step 2: 3000 rpm for 60 s) onto ITO substrate and then soft-baked at 120 ℃ for 90 s on the hot plate (EH20B, Lab Tech, Beijing, China). UV light exposure (13 mW\u0026middot;cm\u003csup\u003e\u0026minus;\u0026thinsp;2\u003c/sup\u003e for 13 s) was performed using an aligner (URE-2000/35, Institute of Optics and Electronics, Chengdu, China) with a chrome mask with designed patterns, and then the substrates were submerged in a developer (0.5 wt% KOH) for 90 s. Afterwards, it was cleaned with DI water and blow dried with nitrogen. The patterned photoresist was then hard-baked on the hot plate at 120\u0026deg;C for 30 min. The substrates were then submerged in an acidic etchant (37 wt% HCl: 68 wt% HNO\u003csub\u003e3\u003c/sub\u003e: H\u003csub\u003e2\u003c/sub\u003eO\u0026thinsp;=\u0026thinsp;50: 3: 50, V/V) until the exposed ITO area was fully etched. The photoresist residue was removed by ethanol after cleaned by DI water and then dried by nitrogen blow to obtain the patterned electrode.\u003c/p\u003e \u003cp\u003eThe LC materials were assembled between two glass substrates (\u003cb\u003eSupplementary Fig.\u0026nbsp;1\u003c/b\u003e). First, the bare and patterned ITO electrode was spin-coated with Hyflon (377 nm) to form a stable dielectric protective layer. The upper substrate was made of a Hyflon-coated uniform ITO electrode. The lower substrate was patterned electrode with Hyflon. The cell was assembled by patterned electrode and a bare ITO electrode using a commercial double tape as a spacer. To easily connect the wires, two substrates were controlled in dislocation. Subsequently, the LC cell was filled with 5CB by capillary force at 40\u0026deg;C above the isotropic temperature and then cooled down to the room temperature. Additionally, we sealed the edge using the UV curing to prevent the leakage of LC.\u003c/p\u003e \u003c/div\u003e \u003cdiv id=\"Sec9\" class=\"Section2\"\u003e \u003ch2\u003eSchematic diagram of optical path\u003c/h2\u003e \u003cp\u003e \u003cb\u003eSupplementary Fig.\u0026nbsp;1\u003c/b\u003e depicts the experimental platform to optically characterize the samples. A collimated Gaussian beam is expanded by the beam expander consisting of lens1, pinhole and lens2. After that, it is converted into circularly polarized light by a linear polarizer (LP) and a quarter waveplate (QWP). Finally, the collimated beam reflected by a mirror normally impinges onto the sample placed on the microscope stage. Charge Coupled Device (CCD, Leica DMC 4500) together with a \u0026times;5 magnification objective lens is used to collect the diffraction field of the sample. The blue double arrow represents the moving direction of the stage, and the distance between the surface of NLC layer and the acquired OM image is defined as \u0026ldquo;\u003cem\u003ez\u003c/em\u003e\u0026rdquo; (\u003cb\u003eSupplementary Fig.\u0026nbsp;1\u003c/b\u003e). The diameter and spacing of the patterned electrode are denoted with \u0026ldquo;\u003cem\u003eD\u003c/em\u003e and \u003cem\u003eL\u003c/em\u003e\u0026rdquo; and the pitch is \u0026ldquo;\u003cspan class=\"InlineEquation\"\u003e\u003cspan class=\"mathinline\"\u003e\\(d=D+L\\)\u003c/span\u003e\u003c/span\u003e\u0026rdquo;. The thickness of LC layer is described as \u0026ldquo;\u003cem\u003eH\u003c/em\u003e\u0026rdquo;.\u003c/p\u003e \u003c/div\u003e \u003cdiv id=\"Sec10\" class=\"Section2\"\u003e \u003ch2\u003ePreparation of lithography samples\u003c/h2\u003e \u003cp\u003eThe microscope cover glass and the silicon wafer were cleaned by soaking it in piranha solution (H\u003csub\u003e2\u003c/sub\u003eO\u003csub\u003e2\u003c/sub\u003e: H\u003csub\u003e2\u003c/sub\u003eSO\u003csub\u003e4\u003c/sub\u003e\u0026thinsp;=\u0026thinsp;1: 3), and then rinsed with DI water and blow dried using the nitrogen. The HN-018 photoresist was spin-coated on the glass and silicon wafer: step 1: 500 rpm for 5 s, step 2: 1000 rpm for 65 s for 8 \u0026micro;m thickness, step 1: 500 rpm for 5 s, step 2: 2000 rpm for 65 s for 4 \u0026micro;m thickness, and step 1: 500 rpm for 5 s, step 2: 2500 rpm for 65 s for 3 \u0026micro;m thickness. After that, it was soft-baked at 90 ℃ for 90 s, exposed, developed for 30 s with 0.4 wt% KOH, and then hard-baked at 210 ℃ for 30 min on a hot plate.\u003c/p\u003e \u003c/div\u003e \u003cdiv id=\"Sec11\" class=\"Section2\"\u003e \u003ch2\u003eNumerical methods\u003c/h2\u003e \u003cp\u003eTo simulate the optical properties of the NLC device, the first task is to efficiently calculate the molecular director configuration. According to P. G. de Gennes\u003csup\u003e\u003cspan citationid=\"CR46\" class=\"CitationRef\"\u003e46\u003c/span\u003e\u003c/sup\u003e, the average molecule direction of rod-shaped uniaxial molecule 5CB can be described by its director \u003cem\u003en\u003c/em\u003e (\u003cem\u003en\u003c/em\u003e = -\u003cem\u003en\u003c/em\u003e). Therefore, the Landau-de Gennes\u0026rsquo;s Q tensor is employed to represent the director\u0026rsquo;s configuration and the elastic free energy of NLC. Afterwards, the NLC molecular directors tend to rotate to reduce the overall energy of the system and ultimately rearrange along the electric field lines based on the dielectric anisotropy when a voltage is applied. The total free energy is minimized when the energy of the electric field is competitive with the elastic energy of NLC. The Euler-Lagrange equations are used to solve the director configuration by using the relaxation method based on dynamics\u003csup\u003e\u003cspan citationid=\"CR47\" class=\"CitationRef\"\u003e47\u003c/span\u003e\u003c/sup\u003e. To expedite the calculation process, techniques such as the momentum gradient descent algorithm, the improved successive over relaxation method, the multigrid, and the symmetric boundary conditions are utilized. The formulas of calculation processes refer to the \u003cb\u003esupporting information\u003c/b\u003e.\u003c/p\u003e \u003cp\u003eAfter obtaining the director configuration of NLC molecules between the sandwich electrodes, this information is used to model the device and then simulate the diffraction field using the commercial-available FDTD (Finite-Difference Time-Domain) software. Basically, the model in this study cannot be fully simulated by the FDTD software, due to the heavy computational cost. However, we notice that the light passing through the NLC layer propagates through a uniform and parallel medium of glass and air. In this case, the diffraction pattern can be efficiently simulated using the vectorial Rayleigh-Sommerfeld diffraction formula and fast Fourier transform, which help to greatly reduce the computing resources and run time.\u003c/p\u003e \u003c/div\u003e \u003cdiv id=\"Sec12\" class=\"Section2\"\u003e \u003ch2\u003eMaterials\u003c/h2\u003e \u003cp\u003eIndium-tin-oxide (ITO) coated glass (700 \u0026micro;m, 90\u0026thinsp;\u0026plusmn;\u0026thinsp;10 Ω\u0026middot;sq\u003csup\u003e\u0026minus;\u0026thinsp;1\u003c/sup\u003e, Leaguer Optronics CO., Ltd, Shenzhen, China) was employed as electrode substrates. The 110 \u0026micro;m thickness microscope cover glass (Fisherbrand\u0026reg;) was procured by Thermo Fisher scientific, Germany. P-type (100) 4\u0026Prime; silicon wafers were acquired from Lijing Optoelctronics Co., Ltd. (Suzhou, China). Nematic liquid crystal of 4-cyano-4\u0026rsquo;-pentyl-biphenyl (5CB, T\u003csub\u003eNI\u003c/sub\u003e = 35 ℃; K\u003csub\u003e11\u003c/sub\u003e\u0026thinsp;=\u0026thinsp;6.2, K\u003csub\u003e22\u003c/sub\u003e\u0026thinsp;=\u0026thinsp;3.9, K\u003csub\u003e33\u003c/sub\u003e\u0026thinsp;=\u0026thinsp;8.2 pN; ε\u003csub\u003e‖\u003c/sub\u003e\u0026thinsp;=\u0026thinsp;18.5, ε\u003csub\u003e\u0026perp;\u003c/sub\u003e\u0026thinsp;=\u0026thinsp;7.0; \u003cem\u003en\u003c/em\u003e\u003csub\u003e\u003cem\u003ee\u003c/em\u003e\u003c/sub\u003e = 1.6975, \u003cem\u003en\u003c/em\u003e\u003csub\u003e\u003cem\u003eo\u003c/em\u003e\u003c/sub\u003e = 1.5350) was purchased from J\u0026amp;K Scientific Co., Ltd., China. Hyflon (AD 40 SX 2.5 wt%) was obtained from Solvay (Shanghai) Co., Ltd., China. A negative-type photoresist (HN-018) and positive-type photoresist (SUN-120P) was soured from Suntific Microelectronic Materials Co. Ltd, Weifang, China. KOH and TMAH (Tetramethylammonium hydroxide) were purchased from Aladdin, Shanghai, China. H\u003csub\u003e2\u003c/sub\u003eO\u003csub\u003e2\u003c/sub\u003e, H\u003csub\u003e2\u003c/sub\u003eSO\u003csub\u003e4\u003c/sub\u003e, HCl and HNO\u003csub\u003e3\u003c/sub\u003e was obtained Guangzhou chemical reagent Co., Ltd., Guangzhou, China.\u003c/p\u003e \u003c/div\u003e"},{"header":"Declarations","content":"\u003cp\u003e\u003cstrong\u003eData availability:\u003c/strong\u003e All data are available in the main text or the Supplementary materials.\u003c/p\u003e\n\u003cp\u003e\u003cstrong\u003eAcknowledgments:\u0026nbsp;\u003c/strong\u003eWe acknowledge all lab members for supporter and guidance on this project. We thank Minxing Lu for the characterization of 3D surface topography. We appreciate the financial support from the Special Project for Marine Economy Development of Guangdong Province (GDNRC[2023]26), the Key Project of National Natural Science Foundation of China (No. 12131010), the International Cooperation Base of Infrared Reflection Liquid Crystal Polymers and Device (2015B050501010), Guangzhou Basic and Applied Basic Research Project (202201010531) and the Science and Technology Project of South China Normal University (21KJ05).\u003c/p\u003e\n\u003cp\u003e\u003cstrong\u003eAuthor contributions:\u0026nbsp;\u003c/strong\u003eM.L., R.Y., H.Y. and L.S. proposed and designed all experiments. M.L., R.Y., K.C., H.F., H.L., S.H., H.Y. and L.S. performed the experiments. M.L., R.Y., Z.G., K.C., H.F., H.L., S.H., M.Z., H.Y. and L.S. discussed and analyzed the experimental results as well as the presentation of the results. M.L., Z.G. and H.Y. contributed to the numerical simulation work. M.L., H.F., K.C., H.L., M.Z. and L.S. participated the discussion. M.L., R.Y., H.Y. and L.S. wrote and polished the initial manuscript. All authors took part in formulating and writing toward the finalization of the manuscript.\u003c/p\u003e\n\u003cp\u003e\u003cstrong\u003eCompeting interests:\u003c/strong\u003e All other authors declare that they have no competing interests.\u003c/p\u003e"},{"header":"References","content":"\u003col\u003e\n\u003cli\u003eKim, T., Bae J.-Y., Lee, N. \u0026amp; Cho, H. H. Hierarchical metamaterials for multispectral camouflage of infrared and microwaves. \u003cem\u003eAdv. Funct. Mater.\u003c/em\u003e \u003cstrong\u003e29\u003c/strong\u003e, 1807319 (2019).\u003c/li\u003e\n\u003cli\u003eZhang, H., Wu, J., Fang, D. \u0026amp; Zhang, Y. Hierarchical mechanical metamaterials built with scalable tristable elements for ternary logic operation and amplitude modulation. \u003cem\u003eSci. Adv.\u003c/em\u003e \u003cstrong\u003e7\u003c/strong\u003e, eabf1966 (2021).\u003c/li\u003e\n\u003cli\u003eXie, Y.-Y. et al\u003cem\u003e.\u003c/em\u003e Metasurface-integrated vertical cavity surface-emitting lasers for programmable directional lasing emissions. \u003cem\u003eNat. Nanotechnol\u003c/em\u003e. \u003cstrong\u003e15\u003c/strong\u003e, 125-131 (2020).\u003c/li\u003e\n\u003cli\u003eRun, H. et al. Thermal camouflaging metamaterials. \u003cem\u003eMater. Today\u003c/em\u003e. \u003cstrong\u003e45\u003c/strong\u003e, 120-141 (2021).\u003c/li\u003e\n\u003cli\u003eMurataj, I. et al. Hyperbolic metamaterials via hierarchical block copolymer nanostructures. \u003cem\u003eAdv. Opt. Mater\u003c/em\u003e. \u003cstrong\u003e9\u003c/strong\u003e, 2001933 (2021).\u003c/li\u003e\n\u003cli\u003eBalli, F., Sultan, M., Lami, S. K. \u0026amp; Hastings, J. T. A hybrid achromatic metalens. \u003cem\u003eNat. Commun\u003c/em\u003e. \u003cstrong\u003e11\u003c/strong\u003e, 3892 (2020).\u003c/li\u003e\n\u003cli\u003eFeng, X. et al. Hierarchical metamaterials for laser-infrared-microwave compatible camouflage. \u003cem\u003eOpt. Express\u003c/em\u003e. \u003cstrong\u003e28\u003c/strong\u003e, 9445-9453 (2020).\u003c/li\u003e\n\u003cli\u003eWeiner, M., Ni, X., Li, M., Alu, A. \u0026amp; Khanikaev, A. B. Demonstration of a third-order hierarchy of topological states in a three-dimensional acoustic metamaterial. \u003cem\u003eSci. Adv\u003c/em\u003e. \u003cstrong\u003e6\u003c/strong\u003e, eaay4166 (2020).\u003c/li\u003e\n\u003cli\u003eDudek, K. K., Martinez, J. A. I., Ulliac, G. \u0026amp; Kadic, M. Micro-scale auxetic hierarchical mechanical metamaterials for shape morphing. \u003cem\u003eAdv. Mater\u003c/em\u003e. \u003cstrong\u003e34\u003c/strong\u003e, 2110115 (2022).\u003c/li\u003e\n\u003cli\u003eYu, X., Zhou, J., Liang, H., Jiang, Z. \u0026amp; Wu, L. Mechanical metamaterials associated with stiffness, rigidity and compressibility: A brief review. \u003cem\u003eProg. Mater. Sci\u003c/em\u003e. \u003cstrong\u003e94\u003c/strong\u003e, 114-173 (2018).\u003c/li\u003e\n\u003cli\u003eWang, K., Lin, F., Chen, J., Wei, Z., Wei, K. \u0026amp; Yang X. Three-dimensional hierarchical metamaterials incorporating multi-directional programmable thermal expansion. \u003cem\u003eMech. Mater.\u003c/em\u003e \u003cstrong\u003e163\u003c/strong\u003e, 104095 (2021).\u003c/li\u003e\n\u003cli\u003eGan, Z., Cao, Y., Evans, R. A. \u0026amp; Gu, M. Three-dimensional deep sub-diffraction optical beam lithography with 9 nm feature size. \u003cem\u003eNat. Commun\u003c/em\u003e. \u003cstrong\u003e4\u003c/strong\u003e, 2061 (2013).\u003c/li\u003e\n\u003cli\u003eYoon, G., Kim, I., So, S., Mun, J., Kim, M. \u0026amp; Rho, J. Fabrication of three-dimensional suspended, interlayered and hierarchical nanostructures by accuracy-improved electron beam lithography overlay. \u003cem\u003eSci. Rep\u003c/em\u003e. \u003cstrong\u003e7\u003c/strong\u003e, 6668 (2017).\u003c/li\u003e\n\u003cli\u003eOfir, Y., Moran, I. W., Subramani, C., Carter, K. R. \u0026amp; Rotello, V. M. Nanoimprint lithography for functional three-dimensional patterns. \u003cem\u003eAdv. Mater.\u003c/em\u003e \u003cstrong\u003e22\u003c/strong\u003e, 3608-3614 (2010).\u003c/li\u003e\n\u003cli\u003eLi, H., Yu, W., Xu, J., Yang, C., Wang, Y. \u0026amp; Bu, H. Hierarchical structure formation and pattern replication by capillary force lithography. \u003cem\u003eRSC Adv\u003c/em\u003e. \u003cstrong\u003e4\u003c/strong\u003e, 39684-39690 (2014).\u003c/li\u003e\n\u003cli\u003eZhou, X. \u0026amp; Liu, C.-J. Three-dimensional printing for catalytic applications: current status and perspectives. \u003cem\u003eAdv. Funct. Mater\u003c/em\u003e.\u003cstrong\u003e 27\u003c/strong\u003e, 1701134 (2017).\u003c/li\u003e\n\u003cli\u003eKawata, S., Sun, H. B., Tanaka, T. \u0026amp; Takada, K. Finer features for functional microdevices - Micromachines can be created with higher resolution using two-photon absorption. \u003cem\u003eNature\u003c/em\u003e \u003cstrong\u003e412\u003c/strong\u003e, 697-698 (2001).\u003c/li\u003e\n\u003cli\u003eHarinarayana, V. \u0026amp; Shin, Y. C. Two-photon lithography for three-dimensional fabrication in micro/nanoscale regime: A comprehensive review. \u003cem\u003eOpt Laser Technol\u003c/em\u003e. \u003cstrong\u003e142\u003c/strong\u003e, 107180 (2021).\u003c/li\u003e\n\u003cli\u003eMyers, B. D. \u0026amp; Dravid, V. P. Variable pressure electron beam lithography (VP-\u003cem\u003ee\u003c/em\u003eBL): A new tool for direct patterning of nanometer-scale features on substrates with low electrical conductivity. \u003cem\u003eNano Lett\u003c/em\u003e. \u003cstrong\u003e6\u003c/strong\u003e, 963-968 (2006).\u003c/li\u003e\n\u003cli\u003eGuo, L. J. Nanoimprint lithography: methods and material requirements. \u003cem\u003eAdv. Mater\u003c/em\u003e. \u003cstrong\u003e19\u003c/strong\u003e, 495-513 (2007).\u003c/li\u003e\n\u003cli\u003eCai, Y., Zhao, Z., Chen, J., Yang, T. \u0026amp; Cremer, P. S. Deflected capillary force lithography. \u003cem\u003eACS Nano\u003c/em\u003e \u003cstrong\u003e6\u003c/strong\u003e, 1548-1556 (2012).\u003c/li\u003e\n\u003cli\u003eLigon, S. C., Liska, R., Stampfl, J., Gurr, M. \u0026amp; Muelhaupt, R. Polymers for 3D printing and customized additive manufacturing. \u003cem\u003eChem. Rev\u003c/em\u003e. \u003cstrong\u003e117\u003c/strong\u003e, 10212-10290 (2017).\u003c/li\u003e\n\u003cli\u003eChen, Y., Yang, X. \u0026amp; Gao, J. 3D Janus plasmonic helical nanoapertures for polarization-encrypted data storage. \u003cem\u003eLight Sci. Appl\u003c/em\u003e. \u003cstrong\u003e8\u003c/strong\u003e, 45 (2019).\u003c/li\u003e\n\u003cli\u003eKo, T.-J. et al. Single-step plasma-induced hierarchical structures for tunable water adhesion. \u003cem\u003eSci. Rep\u003c/em\u003e. \u003cstrong\u003e10\u003c/strong\u003e, 874 (2020).\u003c/li\u003e\n\u003cli\u003eEckel, Z. C., Zhou, C., Martin, J. H., Jacobsen, A. J., Carter, W. B. \u0026amp; Schaedler, T. A. Additive manufacturing of polymer-derived ceramics. \u003cem\u003eScience\u003c/em\u003e \u003cstrong\u003e351\u003c/strong\u003e, 58-62 (2016).\u003c/li\u003e\n\u003cli\u003eAubert, T., Huang, J.-Y., Ma, K., Hanrath, T. \u0026amp; Wiesner, U. Porous cage-derived nanomaterial inks for direct and internal three-dimensional printing. \u003cem\u003eNat. Commun\u003c/em\u003e. \u003cstrong\u003e11\u003c/strong\u003e, 4695 (2020).\u003c/li\u003e\n\u003cli\u003eLiu, N., Guo, H., Fu, L., Kaiser, S., Schweizer, H. \u0026amp; Giessen, H. Three-dimensional photonic metamaterials at optical frequencies. \u003cem\u003eNat. Mater\u003c/em\u003e. \u003cstrong\u003e7\u003c/strong\u003e, 31-37 (2008).\u003c/li\u003e\n\u003cli\u003eXu, X. et al. Multiple-patterning nanosphere lithography for fabricating periodic three-dimensional hierarchical nanostructures. \u003cem\u003eACS Nano\u003c/em\u003e \u003cstrong\u003e11\u003c/strong\u003e, 10384-10391 (2017).\u003c/li\u003e\n\u003cli\u003eChoi, S. \u0026amp; Park, J.-K. Two-step photolithography to fabricate multilevel microchannels. \u003cem\u003eBiomicrofluidics\u003c/em\u003e \u003cstrong\u003e4\u003c/strong\u003e, 046503 (2010).\u003c/li\u003e\n\u003cli\u003eCho, H. et al. Multiplex lithography for multilevel multiscale architectures and its application to polymer electrolyte membrane fuel cell. \u003cem\u003eNat. Commun\u003c/em\u003e. \u003cstrong\u003e6\u003c/strong\u003e, 8484 (2015).\u003c/li\u003e\n\u003cli\u003eClerc, M. G., Kowalczyk, M. \u0026amp; Zambra, V. Topological transitions in an oscillatory driven liquid crystal cell. \u003cem\u003eSci. Rep\u003c/em\u003e. \u003cstrong\u003e10\u003c/strong\u003e, 19324 (2020).\u003c/li\u003e\n\u003cli\u003eLi, Y.-L. et al. Tunable liquid crystal grating based holographic 3D display system with wide viewing angle and large size. \u003cem\u003eLight Sci. Appl\u003c/em\u003e. \u003cstrong\u003e11\u003c/strong\u003e, 188 (2022).\u003c/li\u003e\n\u003cli\u003ePark, J., Won, K. \u0026amp; Kim, Y. Liquid crystal between two distributed Bragg reflectors enables multispectral small-pitch spatial light modulator. \u003cem\u003eLight Sci. Appl\u003c/em\u003e. \u003cstrong\u003e11\u003c/strong\u003e, 210 (2022).\u003c/li\u003e\n\u003cli\u003eKim, D. S., Copar, S., Tkalec, U. \u0026amp; Yoon, D. K. Mosaics of topological defects in micropatterned liquid crystal textures. \u003cem\u003eSci. Adv\u003c/em\u003e. \u003cstrong\u003e4\u003c/strong\u003e, eaau8064 (2018).\u003c/li\u003e\n\u003cli\u003eYuan, Y., Liu, Q., Senyuk, B. \u0026amp; Smalyukh, I. I. Elastic colloidal monopoles and reconfigurable self-assembly in liquid crystals. \u003cem\u003eNature\u003c/em\u003e \u003cstrong\u003e570\u003c/strong\u003e, 214-218 (2019).\u003c/li\u003e\n\u003cli\u003eZola, R. S., Bisoyi, H. K., Wang, H., Urbas, A. M., Bunning, T. J. \u0026amp; Li, Q. Dynamic control of light direction enabled by stimuli-responsive liquid crystal gratings. \u003cem\u003eAdv. Mater\u003c/em\u003e. \u003cstrong\u003e31\u003c/strong\u003e, 1806172 (2019).\u003c/li\u003e\n\u003cli\u003ePeddireddy, K., Copar, S., Le, K. V., Musevi, I., Bahr, C. \u0026amp; Jampani, V. S. R. Self-shaping liquid crystal droplets by balancing bulk elasticity and interfacial tension. \u003cem\u003eProc. Natl. Acad. Sci. U.S.A\u003c/em\u003e. \u003cstrong\u003e118\u003c/strong\u003e, e2011174118 (2021).\u003c/li\u003e\n\u003cli\u003eNi, J. et al. Three-dimensional chiral microstructures fabricated by structured optical vortices in isotropic material. \u003cem\u003eLight Sci. Appl\u003c/em\u003e. \u003cstrong\u003e6\u003c/strong\u003e, e17011 (2017).\u003c/li\u003e\n\u003cli\u003eKamal, W. et al. Spatially patterned polymer dispersed liquid crystals for image-integrated smart windows. \u003cem\u003eAdv. Opt. Mater\u003c/em\u003e. \u003cstrong\u003e10\u003c/strong\u003e, 2101748 (2022).\u003c/li\u003e\n\u003cli\u003eShin, Y., Jiang, J., Qin, G., Wang, Q., Zhou, Z. \u0026amp; Yang, D.-K. Patterned waveguide liquid crystal displays. \u003cem\u003eRSC Adv\u003c/em\u003e. \u003cstrong\u003e10\u003c/strong\u003e, 41693-41702 (2020).\u003c/li\u003e\n\u003cli\u003eRodrigues, J. S., Mendes, C. V. C., Fonseca, E. J. S. \u0026amp; Jesus-Silva, A. J. Talbot effect in optical lattices with topological charge. \u003cem\u003eOpt. Lett\u003c/em\u003e. \u003cstrong\u003e42\u003c/strong\u003e, 3944-3947 (2017).\u003c/li\u003e\n\u003cli\u003ePan, R.-P., Hsieh, C.-F., Pan, C.-L. \u0026amp; Chen, C.-Y. Temperature-dependent optical constants and birefringence of nematic liquid crystal 5CB in the terahertz frequency range. \u003cem\u003eJ. Appl. Phys\u003c/em\u003e. \u003cstrong\u003e103\u003c/strong\u003e, 093523 (2008).\u003c/li\u003e\n\u003cli\u003eZheng, H., Zhou, Y., Ugwu, C. F., Du, A., Kravchenko, I. I. \u0026amp; Valentine, J. G. Large-scale metasurfaces based on grayscale nanosphere lithography. \u003cem\u003eACS Photonics\u003c/em\u003e \u003cstrong\u003e8\u003c/strong\u003e, 1824-1831 (2021).\u003c/li\u003e\n\u003cli\u003eChen, H. et al. Vertically aligned InGaN nanowire arrays on pyramid textured Si (100): A 3D arrayed light trapping structure for photoelectrocatalytic water splitting. \u003cem\u003eChem. Eng. J.\u003c/em\u003e \u003cstrong\u003e406\u003c/strong\u003e,126757 (2021).\u003c/li\u003e\n\u003cli\u003eTong, R., Li, C., Ma, S., Liu, X., Zou, S. \u0026amp; Liu, D. Upright pyramids vs. inverted pyramids surface textures: a comparative investigation on the electrical properties of PERC solar cells. \u003cem\u003eJ. Mater. Sci. Mater. Electron.\u003c/em\u003e \u003cstrong\u003e34\u003c/strong\u003e, 54 (2023).\u003c/li\u003e\n\u003cli\u003eGennes, P. G. \u0026amp; Prost, J. \u003cem\u003eThe Physics of Liquid Crystals\u003c/em\u003e (Oxford Univ. Press, Oxford, 1993).\u003c/li\u003e\n\u003cli\u003eXiong, J., Chen, R. \u0026amp; Wu, S.-T. Device simulation of liquid crystal polarization gratings. \u003cem\u003eOpt. Express\u003c/em\u003e. \u003cstrong\u003e27\u003c/strong\u003e, 18102-18112 (2019).\u003c/li\u003e\n\u003c/ol\u003e"}],"fulltextSource":"","fullText":"","funders":[],"hasAdminPriorityOnWorkflow":false,"hasManuscriptDocX":true,"hasOptedInToPreprint":true,"hasPassedJournalQc":"","hasAnyPriority":true,"hideJournal":false,"highlight":"","institution":"","isAcceptedByJournal":true,"isAuthorSuppliedPdf":false,"isDeskRejected":"","isHiddenFromSearch":false,"isInQc":false,"isInWorkflow":false,"isPdf":false,"isPdfUpToDate":true,"isWithdrawnOrRetracted":false,"journal":{"display":true,"email":"[email protected]","identity":"nature-portfolio","isNatureJournal":true,"hasQc":false,"allowDirectSubmit":false,"externalIdentity":"","sideBox":"","snPcode":"","submissionUrl":"","title":"Nature Portfolio","twitterHandle":"","acdcEnabled":false,"dfaEnabled":false,"editorialSystem":"ejp","reportingPortfolio":"","inReviewEnabled":true,"inReviewRevisionsEnabled":false},"keywords":"","lastPublishedDoi":"10.21203/rs.3.rs-3992476/v1","lastPublishedDoiUrl":"https://doi.org/10.21203/rs.3.rs-3992476/v1","license":{"name":"CC BY 4.0","url":"https://creativecommons.org/licenses/by/4.0/"},"manuscriptAbstract":"\u003cp\u003eLithography technology is a powerful tool for preparing complex microstructures through projecting the patterns of static templates with permanent features onto samples. To simplify fabrication and alignment processes, dynamic photomask for multiple configurations preparation becomes increasingly noteworthy. Hereby, we report a dynamic photomask by assembling the electrically stimulated nematic liquid crystal (NLC) into multifarious architectures. We demonstrate that these architectures give rise to reconfigurable and switchable diffraction patterns via electrically modulating the hybrid phase arising from the NLC molecules. These electrically configurable diffraction patterns are adopted as metamask to produce multiple microstructures with height gradients in one-step exposure and hierarchical microstructures through multiple in-situ exposures using standard photolithography. The fabricated pattern has feature size about 3.2 times smaller than the electrode pattern and can be transferred onto silicon wafer via etching. This strategy can be extended to design diverse microstructures with great flexibility and controllability, offers a promising avenue for fabricating metamaterials via complex structures with simplified lithography processes.\u003c/p\u003e","manuscriptTitle":"Dynamic photomask directed lithography based on electrically stimulated nematic liquid crystal architectures","msid":"","msnumber":"","nonDraftVersions":[{"code":1,"date":"2024-02-29 05:42:13","doi":"10.21203/rs.3.rs-3992476/v1","editorialEvents":[],"status":"published","journal":{"display":true,"email":"[email protected]","identity":"nature-communications","isNatureJournal":true,"hasQc":false,"allowDirectSubmit":false,"externalIdentity":"NCOMMS","sideBox":"Learn more about [Nature Communications](http://www.nature.com/ncomms/)","snPcode":"","submissionUrl":"https://mts-ncomms.nature.com/","title":"Nature Communications","twitterHandle":"","acdcEnabled":true,"dfaEnabled":true,"editorialSystem":"ejp","reportingPortfolio":"Nature Communications","inReviewEnabled":true,"inReviewRevisionsEnabled":false}}],"origin":"","ownerIdentity":"3d1f6324-498b-498a-b313-e4e6a6a853c6","owner":[],"postedDate":"February 29th, 2024","published":true,"recentEditorialEvents":[],"rejectedJournal":[],"revision":"","amendment":"","status":"published-in-journal","subjectAreas":[{"id":29033593,"name":"Physical sciences/Physics/Applied physics"},{"id":29033594,"name":"Physical sciences/Physics/Condensed-matter physics"},{"id":29033595,"name":"Physical sciences/Physics/Optical physics"}],"tags":[],"updatedAt":"2024-10-31T07:07:36+00:00","versionOfRecord":{"articleIdentity":"rs-3992476","link":"https://doi.org/10.1038/s41467-024-53530-9","journal":{"identity":"nature-communications","isVorOnly":false,"title":"Nature Communications"},"publishedOn":"2024-10-30 04:00:00","publishedOnDateReadable":"October 30th, 2024"},"versionCreatedAt":"2024-02-29 05:42:13","video":"","vorDoi":"10.1038/s41467-024-53530-9","vorDoiUrl":"https://doi.org/10.1038/s41467-024-53530-9","workflowStages":[]},"version":"v1","identity":"rs-3992476","journalConfig":"researchsquare"},"__N_SSP":true},"page":"/article/[identity]/[[...version]]","query":{"redirect":"/article/rs-3992476","identity":"rs-3992476","version":["v1"]},"buildId":"qtupq5eGEP_6zYnWcrvyt","isFallback":false,"isExperimentalCompile":false,"dynamicIds":[84888],"gssp":true,"scriptLoader":[]}