Dynamically Reconfigurable Polarization in Elastomeric Semiconductors for Stretchable Chiroptoelectronics

Dynamically Reconfigurable Polarization in Elastomeric Semiconductors for Stretchable Chiroptoelectronics | 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 Dynamically Reconfigurable Polarization in Elastomeric Semiconductors for Stretchable Chiroptoelectronics Jin Young Oh, Ngoc Thanh Phuong Vo, Tae Uk Nam, Min Woo Jeong, and 8 more This is a preprint; it has not been peer reviewed by a journal. https://doi.org/ 10.21203/rs.3.rs-7457973/v1 This work is licensed under a CC BY 4.0 License Status: Under Review Version 1 posted You are reading this latest preprint version Abstract Stretchable optoelectronics capable of dynamically controlling and detecting circularly polarized light offer transformative potential for wearable optoelectronic computing, biomimetic sensing, and photonic communication. However, conventional polarization-sensitive materials based on rigid birefringent optical crystals or chiral organic compounds inherently lack mechanical adaptability and reversible polarization tunability. Here, we introduce a mechanically robust, stretchable composite based on alignment-controllable semiconducting polymer nanofibers embedded in an elastomer matrix, which exhibits dynamically tunable optical activity through mechanical deformation and/or angular layer assembly. By stacking individual layers at controlled twist angles, we achieve highly sensitive chiroptical detection in the near-infrared range even under mechanical deformation (up to 50 % uniaxial and 30 % biaxial strain) for stretchable optoelectronics. Furthermore, our devices demonstrate reliable optoelectrical performance with high reproducibility under repeated stretching cycling, maintaining polarization-selective transistor functionality and enabling mechanically programmable optical logic gates (AND, XNOR). Our findings establish a transformative paradigm for mechanically adaptive chiroptoelectronics, enabling skin-integrated photonic sensing and computing. Physical sciences/Optics and photonics/Optical materials and structures/Nanowires Physical sciences/Materials science/Materials for devices/Sensors and biosensors Physical sciences/Nanoscience and technology/Nanoscale materials/Nanowires Physical sciences/Physics/Electronics, photonics and device physics/Electronic and spintronic devices Figures Figure 1 Figure 2 Figure 3 Figure 4 Introduction Controlling and analyzing the polarization states of light is essential for a wide range of optical applications, including displays, spectroscopy, machine vision, and quantum optics. [1-3] For example, liquid crystals have revolutionized display optoelectronic technologies by enabling polarization modulation of anisotropic molecules through electric fields, which control both brightness and color via engineered optical filters, resulting in improved color expression and faster response times. In spectroscopy and photonic devices, photoelastic and acousto-optic modulators play a crucial role in processing polarimetric information. [4] They enable coherence and interference between beams, support high repetition rates from a few hundred kilohertz (kHz) to several megahertz (MHz) for signal modulation, and enhance signal-to-noise ratios through lock-in amplification. [5] However, most polarization modulators are based on rigid optical crystals or fixed optoelectronic devices, rendering them unsuitable for applications such as stretchable photodetectors and reconfigurable bionic artificial eyes. Moreover, the modulation capability of such optical crystals is inherently limited by the deterministic nature of crystalline birefringence, typically allowing only simple polarization switching, such as from vertical to horizontal or from linear to circular. [6,7] Even liquid crystals face intrinsic limitations, as their polarization performance strongly depends on the surface properties of alignment layers and the specific orientation of applied electric fields. Consequently, to realize emerging photonic applications such as biomimetic artificial eyes and deformable optics, it is crucial to develop materials that offer dynamically tunable optical anisotropy and polarization states. [8,9] Flexible optoelectronic systems, such as polarization-resolved chiral-responsive devices, require not only optical filters selective to angular momentum but also stretchable photodetectors capable of mechanical deformation. [10] Recent studies have pursued enantioselective devices by integrating chiral metasurfaces with various organic and inorganic semiconductors. [11,12] Examples include chiral perovskite nanostructures and helicoidal nanoparticles interfaced with transparent conductive metal oxides for circularly polarized light (CPL) detection. [13-16] Furthermore, chiral heterostructures incorporating carbon nanotubes have shown promise for CPL-based neuromorphic memory and pattern recognition. [17-19] Organic molecules, including helicenes, perylene diimide-fused helicenes, (R)- or (S)-1-phenylethylamine, DPA, fullerene, 1,1′-binaphthyl–2,2′-diamine, and cellulose nanocrystals, have also been integrated into organic field-effect transistor (OFET) architectures to achieve CPL photodetection. [20-26] However, these approaches inherently lack mechanical stretchability, as they predominantly rely on rigid organic crystals or inorganic thin-film architectures. Crucially, they also lack dynamic polarization modulation capabilities, specifically the ability to reversibly reconfigure polarization states. This fundamental limitation significantly constrains their potential use in next-generation technologies, such as biomimetic polarization-resolved artificial eyes, stretchable complementary metal-oxide-semiconductor (CMOS) photodetectors, and soft light detection and ranging (LiDAR) systems for advanced humanoid robotics. [27] Here, we present an elastomeric semiconductor composite enabling dynamically reconfigurable polarization and robust mechanical stretchability for chiroptoelectronics. This composite consists of semiconducting polymer nanofibers (DPPT-TT, poly(2,5-bis(2-octyldodecyl)-3,6-di(thiophen-2-yl)diketopyrrolo[3,4-c]pyrrole-1,4-dione-alt-thieno[3,2-b]thiophene) embedded within an elastomeric matrix (SEBS, polystyrene-block-poly(ethylene-ran-butylene)-block-polystyrene), forming a blend film capable of reversible optical polarization encoding via mechanical deformation and electrical field modulation ( Figure 1 ). This molecularly blended film is optically polarization-writable, electrically field-tunable, and highly stretchable. Furthermore, when stacked, the films exhibit interlayer optical and electronic hybridization while retaining their mechanical stretchability. Mechanically Programmable Alignment of Semiconducting Polymer Nanofibers for Stretchable Optoelectronics Figure 1a shows a schematic illustration of the alignment mechanism of DPPT-TT polymer nanofibers embedded within an elastomeric SEBS matrix, achieved through controlled compressive strain. The degree of nanofiber alignment is systematically regulated by adjusting the pre-strain level of a poly(dimethylsiloxane) (PDMS) stamp ( Supplementary Fig. 1 ). Figures 1b-c and Movie S1, S2 present real-time LiDAR imaging, revealing strain-induced linear polarization in the aligned nanofiber blend films. These optoelectronically integrated films demonstrate pronounced linear dichroism (LD) under uniaxial stretching ( Fig. 1c ) and exhibit circular dichroism (CD) when configured as multilayered stacks with precisely controlled interlayer twist angles (Bouligand structures, Fig. 1d ). Such multilayer Bouligand structures display isotropic reflectance under linearly polarized illumination at a near-infrared wavelength (860 nm), clearly contrasting with the anisotropic response seen in single-layer stretched films. The uniform reflectance across the multilayers indicates a homogeneous distribution of circular polarization within the stacked architecture. The optical properties of the composite film primarily originate from strain-induced nanofiber alignment. Initially, DPPT-TT nanofibers spontaneously form randomly oriented networks within the SEBS elastomer through nanoconfined phase separation, driven by strong intermolecular π–π interactions ( Supplementary Fig. 2 ). [28-30] Upon applying compressive strain, these nanofibers uniformly align perpendicular to the strain direction, significantly decreasing inter-fiber spacing, as directly observed by phase-mode atomic force microscopy (AFM) ( Fig. 1e and Supplementary Figs. 3,4 ). Cross-polarized optical microscopy (inset Fig. 1f , Supplementary Fig. 5 ) further confirms uniform nanofiber alignment throughout the films. The degree of alignment, quantified by a two-dimensional order parameter (S 2D ), increases linearly with applied compressive strain ( Fig. 1f ) and is fully reversible upon strain release, restoring the nanofibers to their original random orientation. Aligned composite films exhibit linear dichroism ratios strongly correlated with S 2D under compressive strain ( Fig. 1g , Supplementary Fig. 6 ). Grazing-incidence X-ray diffraction (GIXRD) analyses demonstrate that nanofiber alignment induced by 50% compressive strain correlates directly with preferential molecular orientations in crystalline domains, characterized by prominent (h00) reflections along the Q xy direction ( Fig. 1h , Supplementary Fig. 7 ). [31] Enhanced diffraction intensities occur when the incident X-ray beam is oriented parallel (0°) to the aligned nanofibers rather than perpendicular (90°), confirming highly oriented crystalline domains ( Supplementary Fig. 8 ). Strain-induced nanofiber alignment imparts significant anisotropy not only optically but also electrically, as demonstrated in organic field-effect transistors (OFETs) ( Supplementary Fig. 9 ). OFET channels were defined parallel (∥) or perpendicular (⊥) to the nanofiber alignment axis ( Fig. 1i,j ). Compared to the pristine device (randomly oriented DPPT-TT nanofibers, μ eff = 0.40 cm²/V·s), devices with nanofibers aligned at 50% strain parallel to the charge transport direction exhibited more than twofold enhanced field-effect mobility (0.9 cm²/V·s). Conversely, mobility decreased approximately by half (0.20 cm²/V·s) in the perpendicular orientation, while maintaining consistently low leakage currents (~10 -10 A) and high on/off current ratios (>10 4 ) ( Fig. 1k , Supporting Note 4 , Supplementary Figs. 13-16 ). These differences primarily stem from alignment-induced formation of efficient charge percolation pathways along the current direction, as further supported by reductions in activation energy (E A ), Urbach energy (E U ), and contact resistance (R C ) ( Supporting Note 5 ). Moreover, our devices demonstrate outstanding mechanical durability, retaining stable mobility, drain current, and optical anisotropy even after 10,000 cycles of repeated stretching at 100% tensile strain ( Fig. 1l , Supplementary Figs. 24-26 ). Multilayer Bouligand Structures for Chiral Optoelectronic Detection and Polarization-Encoding Expanding on our findings from single-layer films, we explored multilayered structures composed of individually aligned blend films stacked at precise twist angles. These multilayers exhibit emergent chiral optical and electrical characteristics originating explicitly from controlled interlayer twist angles rather than cumulative linear polarization. To investigate these chiroptical properties, we fabricated OFETs incorporating helically stacked blend films arranged into Bouligand structures, with each successive layer rotated by 45° relative to the underlying layer ( Fig. 2a ). Each aligned film (80 nm thickness) was prepared by transferring a nanofiber-aligned polymer layer from a pre-strained (100% tensile) PDMS stamp onto an elastomeric SEBS substrate (0.2 mm thick). Multilayer structures (2-4 layers) were constructed sequentially with precisely defined twist orientations to left-handed ( LH ) and right-handed ( RH ) directions to form robust, electrically interconnected assemblies. The helically stacked films showed distinct circular dichroism (CD) peaks near 750 nm and 850 nm, corresponding respectively to H- and J-type molecular aggregations within DPPT-TT semiconductors ( Fig. 2b ; Supplementary Fig. 27 ). [32-34] Single-layer films exhibited negligible CD signals, whereas bilayer stacks displayed pronounced mirror-symmetric CD absorption bands near 850 nm, indicating hybridized chiral electronic states. As layer number increased, CD intensity progressively amplified to 1,500 mdeg, corresponding to a substantial dissymmetry factor of absorbance (g-factor ≈ 0.1), defined as ), where and represent the absorption under left ( L -) and right ( R -) CPL, respectively ( Fig. 2c ). A slight redshift of the main absorption peak to ~870 nm further confirmed enhanced π-conjugation and exciton coupling across the layers. Neither pure SEBS nor neat DPPT-TT films exhibited intrinsic chiroptical activity, verifying that the observed chirality emerged solely from the ordered alignment and interlayer hybridization of nanofibers rather than inherent molecular chirality ( Supplementary Figs. 28,29 ). Multilayer structures and large-scale solid samples often exhibit apparent CD behavior due to compositional optical effects arising from interactions between layers with distinctly different optical properties, such as dichroism and birefringence. [35] Angular-dependent CD measurements showed negligible variation upon azimuthal angle rotation and reversed illumination direction, as confirmed by Mueller matrix symmetry conditions (M 03 = M 30 ), strongly supporting genuine structural chirality from the stacked architecture ( Fig. 2d,e and Supplementary Figs. 30–32 ). Our multilayered films demonstrate chiral, gate-tunable transistor functionality achievable only when the nanofibers exhibit both strong optical anisotropy and efficient three-dimensional charge-transport pathways, characteristics not attainable with conventional chiral materials such as linear optically active chromophores, Langmuir-Blodgett films, or chiral nanoparticle assemblies. [36] Strong exciton coupling involving π-π transitions and charge-transfer states results in pronounced polarization-dependent photocurrents under CPL illumination. Stacked chiroptoelectronic transistors displayed significant stereoselective enhancement of off-state current upon illumination with co-polarized CPL, attributed to enhanced photocarrier generation in the transistor channel ( Fig. 2f and Supplementary Fig. 33 ). Devices comprising up to four stacked layers consistently exhibited clear trends in on/off currents under L- and R- CPL illumination, maintaining over 10⁴ on/off current ratios despite substantial modulation of the off-state current ( Fig. 2f ). Additionally, four-layer Bouligand structures showed isotropic optical responses, substantially minimizing azimuthal-angle dependence of transistor characteristics ( Fig. 2g,h ). Beyond fundamental CPL detection, the multilayered Bouligand films provided helicity-selective electronic outputs enabling advanced polarization-based digital functionalities. Unlike conventional CPL photodetectors limited to binary polarization detection ( L- or R- CP), our devices continuously differentiate polarization states ranging from linear to elliptical to circular, highlighting their applicability for real-time polarization-resolved computing and secure optical communication. Moreover, four-layer stacked films demonstrated direct extraction of retarder angles by monitoring transistor drain current at the off-state (V G = 10 V), under continuously varying ( Fig. 2i ) and digitally randomized polarization inputs ( Fig. 2j and Supplementary Fig. 34 ). This capability strongly suggests potential applications in advanced data transmission and secure optical encryption, analogous to emerging infrared-based optical communication technologies such as Li-Fi. Mechanically Robust Multilayer Bouligand-Structured Semiconducting Elastomers for Stretchable Chiral Photodetection A fundamental advantage of elastomeric semiconductor films is their inherent softness and elasticity, suited for emerging stretchable chiroptoelectronic applications. Unlike conventional rigid optical crystals, our elastomeric composite closely matches the elastic modulus of human skin, demonstrating exceptional mechanical resilience and flexibility. To quantitatively assess this capability, we investigated LH and RH multilayer (4-layer) Bouligand-structured OFETs under substantial mechanical deformation ( Fig. 3 and Supplementary Figs. 35,36 ). The key optical and electrical properties remained robust under both uniaxial (up to 50%) and biaxial (up to 30%) tensile strains. Even at 30% biaxial strain, differences in the off-state current responses to L- and R- CPL were nearly identical to those in unstrained devices, confirming reliable chirality-selective detection under complex mechanical environments ( Supplementary Figs. 37-41 ). The CD measurements further verified the mechanical stability of chiral optical properties. Under 50% uniaxial strain, CD intensity decreased modestly (~28%), accompanied by a 99 nm blue shift, while under 30% biaxial strain, CD intensity decreased by approximately 22% with a 32 nm blue shift ( Fig. 3a and Supplementary Figs. 42-44 ). Despite mechanical deformation, the resilience of CD spectra underscores the critical influence of precisely controlled interlayer twist angles in preserving chiroptical responses. These mechanical perturbations resulted only in minor (~10% for LH and ~15% for RH configurations) reductions in the dissymmetry factor (g ph ), further validating the mechanical and optical robustness of the composites ( Fig. 3b and Supplementary Fig. 45 ). The primary performance metric of the elastic Bouligand-structured semiconductor is the magnitude of photocurrent differences generated by L- and R- CPL illumination under identical intensities. To quantitatively evaluate sensor performance, we analyzed the sensitivity and linear dynamic range (LDR) by monitoring photocurrent differences as a function of incident light intensity, both before and after mechanical deformation ( Fig. 3c,d and Supplementary Figs. 46,47 ). The pristine devices showed a linear dynamic range of 0.645-1.504 mW/cm² and sensitivity of approximately 27-31 cm²/mW. These key metrics remained largely unaffected by significant uniaxial (50%) and biaxial (30%) tensile strains, demonstrating exceptional mechanical reliability and stable performance ( Fig. 3e and Supplementary Table 2 ). To gain further insight into dynamic optoelectronic stability, we investigated the time-resolved photocurrent responses of the OFET devices. Under cyclic illumination with alternating L- and R- CPL, pristine devices consistently exhibited distinct and stable photocurrent states corresponding to co- and cross-polarized conditions, respectively. The response and recovery times of both RH and LH configurations were measured to be approximately 2.01 ± 0.2 s and 1.08 ± 0.3 s, respectively ( Supplementary Figs. 48,49 ). These rapid response characteristics remained stable under significant mechanical strain conditions (50% uniaxial and 30% biaxial), demonstrating exceptional dynamic robustness ( Fig. 3f-h ). Collectively, these results confirm that the controlled interlayer twist angle predominantly governs the enantioselective optical response of the device, exhibiting superior robustness over uniformly applied mechanical deformation. Mechanically Reconfigurable Chiral Optoelectronics A distinctive feature of this elastomeric semiconductor composite is its distinctive ability to dynamically and reversibly program optical polarization states through mechanical strain, analogous to data writing and erasing processes in electronic memory devices, while simultaneously operating as transistors. Additionally, unlike mechanically reconfigurable films comprising dye or liquid crystal blends with nanomaterials, our material inherently integrates transistor functionality. This versatile capability is realized using a minimal bilayer architecture, wherein the top layer initially consists of randomly oriented nanofibers, while the bottom layer is pre-aligned through 50% compressive strain at a 45° orientation relative to the substrate ( Fig. 4a ). Upon applying 50% tensile strain, nanofibers in the top isotropic layer directionally align, while the pre-aligned bottom layer remains effectively stable ( Supplementary Fig. 50 ). Leveraging this design, we fabricated a 5×5 active-matrix transistor array capable of selectively detecting L- and R- CPL by simply adjusting the direction of applied mechanical strain ( Fig. 4b and Supplementary Fig. 51 ). All pixel transistors exhibited highly uniform, hysteresis-free electrical responses to CPL illumination, preserving stable performance even after repeated uniaxial stretching cycles up to 50% strain ( Supplementary Fig. 52 ). The CD measurements demonstrated stable optical characteristics, consistently maintaining ~500 mdeg intensity under repeated 25% tensile strain and significantly increasing to approximately ~700 mdeg under 50% tensile strain ( Fig. 4c ; Supplementary Figs. 53,54 ). This enhancement originates from increased molecular ordering and improved intermolecular interactions induced by moderate mechanical strain. Correspondingly, the optoelectronic characteristics exhibited remarkable robustness, comparable to multilayer Bouligand structures. In an unstrained state, transistor arrays showed highly uniform off-current ratios (I LCPL /I RCPL : 1.05; Fig. 4d ). Under mechanical deformation (50% uniaxial strain), the devices demonstrated precise discrimination among linear, elliptical, and circular polarization states, consistently generating reproducible photocurrent signals ( Fig. 4e,f and Supplementary Fig. 55 ). Illumination with CPL matching the mechanically induced chirality significantly enhanced the off-state current, yielding nearly an order-of-magnitude increase compared to illumination with opposite-handed CPL ( Fig. 4g,h and Supplementary Figs. 56-58 ). Importantly, the photocurrent asymmetry, quantified by the dissymmetry factor (g ph = 0.65), remained exceptionally stable through multiple 50% stretching cycles ( Fig. 4i ). Capitalizing on the demonstrated mechanically tunable CPL sensitivity, we further implemented a polarization-sensitive optoelectronic logic gate capable of fundamental logic operations (AND, XNOR) modulated by mechanical deformation and CPL illumination ( Fig. 4j and Supplementary Fig. 59 ). Our experimental protocol systematically translated mechanical and optical stimuli into discrete electrical outputs through three sequential stages ( Fig. 4k ). Initially (Stage 1), baseline off-state currents were established in the unstrained, dark condition. Subsequently (Stage 2), intrinsic polarization sensitivity was evaluated under sequential L- and R-CPL illumination without applied strain. In the final step (Stage 3), applying 50% tensile strain either parallel or perpendicular to the substrate axis set distinct polarization-sensitive axes (+45° or -45°), allowing selective and reproducible photocurrent responses to CPL illumination. Explicit logic gate demonstration involved defining binary inputs based on controlled parameters: mechanical strain (logic '0' = 0%, logic '1' = 50% strain) and CPL illumination intensity (logic '0' = dark, logic '1' = 1.6 mW/cm²). The AND gate exhibited high photocurrent output ('1') only with simultaneous strain and illumination inputs. For the XNOR gate, binary inputs included strain direction (90° as '0', 0° as '1') relative to pre-aligned layers and CPL handedness (LCP as '0', RCP as '1'), producing high output only when inputs matched. All logic input combinations generated accurate and reproducible outputs ( Fig. 4l and Supplementary Table 3 ). An elastomeric semiconductor platform capable of robustly and reversibly encoding chiral optical states, while simultaneously maintaining stable transistor functionality under extensive mechanical deformation. This integrated system-level approach unlocks unprecedented opportunities in stretchable chiroptoelectronics. Methods Materials: Poly(2,5-bis(2-octyldodecyl)-3,6-di(thiophen-2-yl)diketopyrrolo[3,4-c]pyrrole-1,4-dione-alt-thieno[3,2-b]thiophen) (DPPT-TT) (Derthon, M w /M n = 100k/42k) polymer was traded by Derthon. Polystyrene-block-poly(ethylene-ranbutylene)-block-polystyrene (SEBS) was purchased from Asahi Kasei company. Poly(-dimethylsiloxane) (PDMS, Sylgard 184) and its cross-linker were supported by Dow Corning. The PDMS was cured with a ratio of 10:1 (base/cross-linker, w/w) at 65 °C overnight for the transfer printing stamp. Ag (silver, 99.99%, 3–5 mm granule) was purchased from SY SCIENCE. The Trichloro(octadecyl)silane (OTS) solution and diiodomethane were purchased by Sigma Aldrich. Anhydrous chlorobenzene, chloroform, and toluene were purchased by Sigma Aldrich. All chemicals and materials were used without any purification. Device fabrications and characterizations Fully stretchable transistors: Thin film preparation. The semiconductor solution was prepared by dissolving DPPT-TT (0.21 wt%) and SEBS H1062 (S/EB weight ratio of 18/82, 0.49 wt%) with a total of 0.7 wt%, in anhydrous chlorobenzene at 120 °C for 4 h. The solution was spun on an OTS-treated SiO 2 /Si wafer at 1000 rpm for 1 min after filtration with a PTFE-D (0.2 μm) filter (film thickness: 80 nm). The semiconducting film was then annealed at 180 °C for 1 hour. All processes were carried out under an N 2 atmosphere in a glove box with extremely low levels of moisture (H 2 O < 0.01 parts per million (ppm)) and oxygen (O 2 < 0.01 ppm). The SEBS H1052 dielectric solution (S/EB weight ratio of 20/80, 60 mg/mL in toluene) was dissolved at 70 o C for 4 h in ambient condition, then, was spun at 1000 rpm for 1 min (film thickness: 1200 nm) on OTS-treated SiO 2 without any heat treatment. Fully stretchable transistor preparation. The elastomer substrates were prepared by casting SEBS H1062 (100 mg/ml in toluene) onto glass slides to form elastic films with the approximate thickness around 0.2 mm. Ag gate electrode (50 nm thick) was thermally evaporated onto the SEBS substrate at a speed of 0.2 nm/s under high vacuum conditions (below 6.0 × 10 −6 torr). SEBS H1052 dielectric and semiconducting film on OTS-treated SiO 2 were sequentially transferred onto the gate electrode. Finally, the 50 nm-thick source/drain electrodes were evaporated at a rate of 0.2 nm/s using a thermal evaporator one to form the top contact/bottom gate field-effect-transistor structure. The channel length and width were 1000 and 150 μm, respectively. The semiconducting layers were stacked in clockwise direction and counterclockwise direction with 45-degree to the beneath layer in each stacked layer to achieve Bouligand structure. Active-matrix transistor array for logic gate function. All the procedures were identical to the fabrication process of fully stretchable transistors, except for the dielectric film. The dielectric layer with a different concentration (75 mg/ml in toluene, 1.8 μm thick) was used and spin-coated at 1000 rpm for 1 min to achieve a thicker dielectric film to reduce leakage current. Bouligand structure for optical measurements . The semiconducting layers were transferred and stacked in clockwise direction and counterclockwise direction with 45-degree twist angles to the beneath layer on SEBS substrate. Characterization For stabilization of the devices, all devices were aged overnight in an auto-dry desiccator. The electrical characteristics of devices were measured using probe station connected with KEITHLEY 4200 and direct current generator (OWON, P4305) under ambient condition. To maximize photo-response current, a laser at 830 nm was selected with a power density of 1.6 mW/cm² and a beam diameter of 0.2 mm, corresponding to the peak where CD absorption is maximized (Fig. 2b). The capacitances of dielectric were measured using probe station connected with LCR meter (Keysight 4274A). The UV-Vis-Nir and polarized UV-Vis-Nir spectrums were obtained with spectrophotometer (JASCO, V-770). The surface structures and current images were obtained with atomic force microscopy (AFM; Bruker MultiMode 8-HR) under ambient condition. The optical images and polarized optical images obtained with optical microscope (OM; Leica DM4 M). The thickness of the films was obtained with an ellipsometer (WONWOO STRC-2000). Grazing incidence X-ray diffraction (GIXD) patterns of semiconducting thin films were performed on a laboratory beamline system (Xenocs Inc. Xeuss 2.0) with an X‐ray wavelength of 1.54 Å and sample to detector distance of 15 cm. Samples were kept under vacuum to minimize air scattering. The surface energy and contact angle were obtained by PHOENIX-MT(T). The CD spectra was measured using JASCO-815 CD spectrometer with NIR detector from 300nm - 900nm, 0.5msec, 1s D.I.T. and from 700nm - 1100nm, 0.5msec, 1s D.I.T. Declarations Acknowledgments This research was supported by Basic Science Research Program through the National Research Foundation of Korea (NRF) funded by the Ministry of Education (RS-2021-NR061555 and RS-2020-NR049601), GRRC program of Gyeonggi province (GRRCKYUNGHEE2023-B03), the Korea Institute for Advanced of Technology (KIAT) and the Ministry of Trade, Industry & Energy (MOTIE) of the Republic of Korea (RS-2024-00434908 and RS-2025-25435993), and the auspices of the U.S. Department of Energy by Lawrence Livermore National Laboratory under Contract DE-AC52-07NA27344. W.J.C. gratefully acknowledge the LLNL LDRD Program for funding support of this project under No.22-ERD-056. X.G. and G.M. thanks NSF for supporting the morphology characterizations performed in this work under award number CHE-2304969. Author contributions N.T.P.V. and J.Y.O. conceived the study and N.T.P.V., W.C., T.I.L., and J.Y.O. designed the experiments. N.T.P.V. conducted all experiments. N.T.P.V., T.U.N., M.W.J., K.H.J., T.A.N., S.H.P., H.R.C., G.M., X.G., T.I.L., W.C., and J.Y.O. analyzed and discussed the data. N.T.P.V., T.I.L., W.C., and J.Y.O. wrote the manuscript. Competing interests Authors declare that they have no competing interests. Data availability Data are available on request. Correspondence and requests for materials should be addressed to T.I.L., W.J.C., and J.Y.O. Supplementary information The online version contains supplementary material available at https://doi.org/##.#### References Jan, C. M., Lee, Y. H., Wu, K. C. & Lee, C. K. Integrating fault tolerance algorithm and circularly polarized ellipsometer for point-of-care applications. Opt. Express 19 , 5431–5441 (2011). Sherson, J. F. et al. Quantum teleportation between light and matter. Nature 443 , 557–560 (2006). Wagenknecht, C. et al. Experimental demonstration of a heralded entanglement source. Nat. Photon. 4 , 549–552 (2010). Zhang, R., Wen, T., Wang, Y., Wang, Z., & Li, K. 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Mat. 34 , 2305252 (2024). Vo, N.T.P., Nam, T.U. et al. Autonomous self-healing supramolecular polymer transistors for skin electronics. Nat Commun. 15 , 3433 (2024). Xu, J., Wu, H. C. et al. Multi-scale ordering in highly stretchable polymer semiconducting films. Nat. Mater. 18 , 594-601 (2019). Clark, J. et al. Determining exciton bandwidth and film microstructure in polythiophene films using linear absorption spectroscopy. Appl. Phys. Lett. 94 , 163306 (2009). Pace, G. et al. Intrinsically distinct hole and electron transport in conjugated polymers controlled by intra and intermolecular interactions. Nat. Commun. 10 , 5226 (2019). Li, Y., Singh, S. P., & Sonar, P. A high mobility P‐type DPP‐thieno [3, 2‐b] thiophene copolymer for organic thin‐film transistors. Adv. Mater. 22 , 4862-4866 (2010). Kim, Y., Yeom, B. et al. Reconfigurable chiroptical nanocomposites with chirality transfer from the macro-to the nanoscale. Nat. Mater. 15 , 461-468 (2016). Zhang, L., Lu, Q. & Liu, M. Fabrication of chiral Langmuir-Schaefer films from achiral TPPS and amphiphiles through the adsorption at the air/water interface. J. Phys. Chem. B 107 , 2565–2569 (2003). Additional Declarations There is NO Competing Interest. Supplementary Files 20250826SupplementaryInformation.pdf Supplementary Figures MovieS1.mp4 Movie S1 MovieS2.mp4 Movie S2 Cite Share Download PDF Status: Under Review 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. We do this by developing innovative software and high quality services for the global research community. Our growing team is made up of researchers and industry professionals working together to solve the most critical problems facing scientific publishing. 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-7457973","acceptedTermsAndConditions":true,"allowDirectSubmit":false,"archivedVersions":[],"articleType":"Article","associatedPublications":[],"authors":[{"id":591040358,"identity":"323524a0-7755-4982-87e5-1193b7043870","order_by":0,"name":"Jin Young Oh","email":"data:image/png;base64,iVBORw0KGgoAAAANSUhEUgAAAZAAAAAyAQMAAABI0h/eAAAABlBMVEX///8AAABVwtN+AAAACXBIWXMAAA7EAAAOxAGVKw4bAAAAq0lEQVRIiWNgGAWjYBACxgYGNoYPBw7AOERqYZxBkhYgYGPmIUkL84zkY49tztxJbGA//IBx5h5iHDYjLd0458azxAaeNAPGDc+I0pJjJp3z4XBiA0MOA+ODA8RqsQBp4X9DihaGG0AtEkBbNhClpedZmmTPmcPGbRLPDA7OIEaLYXvyMYkfxw7L9vMnP3zYQ5SWCQkQBhsQE6OBgUGenzh1o2AUjIJRMJIBAChPPmnww5LmAAAAAElFTkSuQmCC","orcid":"https://orcid.org/0000-0003-2260-9960","institution":"Kyung Hee University","correspondingAuthor":true,"prefix":"","firstName":"Jin","middleName":"Young","lastName":"Oh","suffix":""},{"id":591040359,"identity":"34211133-6aa6-42e6-9e7e-c866c77f32e9","order_by":1,"name":"Ngoc Thanh Phuong Vo","email":"","orcid":"","institution":"Kyung Hee University","correspondingAuthor":false,"prefix":"","firstName":"Ngoc","middleName":"Thanh Phuong","lastName":"Vo","suffix":""},{"id":591040360,"identity":"b8cfeab4-dd5d-4789-9ad3-2e4f480bbbe9","order_by":2,"name":"Tae Uk Nam","email":"","orcid":"","institution":"Kyung Hee University","correspondingAuthor":false,"prefix":"","firstName":"Tae","middleName":"Uk","lastName":"Nam","suffix":""},{"id":591040361,"identity":"e63710fb-112e-4335-a7bd-0acbb0bf79e3","order_by":3,"name":"Min Woo Jeong","email":"","orcid":"","institution":"Kyung Hee University","correspondingAuthor":false,"prefix":"","firstName":"Min","middleName":"Woo","lastName":"Jeong","suffix":""},{"id":591040362,"identity":"db42fbb4-6ce2-43be-9f98-285b8ecb4d21","order_by":4,"name":"Kyu Ho Jung","email":"","orcid":"","institution":"Kyung Hee University","correspondingAuthor":false,"prefix":"","firstName":"Kyu","middleName":"Ho","lastName":"Jung","suffix":""},{"id":591040363,"identity":"8cb98fdd-64db-43d6-9339-532a5c5b5995","order_by":5,"name":"Thuy An Nguyen","email":"","orcid":"","institution":"Kyung Hee University","correspondingAuthor":false,"prefix":"","firstName":"Thuy","middleName":"An","lastName":"Nguyen","suffix":""},{"id":591040364,"identity":"1ec51981-4709-4818-802b-60b3266d75e1","order_by":6,"name":"Seon Hoo Park","email":"","orcid":"","institution":"Kyung Hee University","correspondingAuthor":false,"prefix":"","firstName":"Seon","middleName":"Hoo","lastName":"Park","suffix":""},{"id":591040365,"identity":"4e0ce1d4-95d8-4535-b94a-e850e5c37505","order_by":7,"name":"Hye Rin Chang","email":"","orcid":"","institution":"Kyung Hee University","correspondingAuthor":false,"prefix":"","firstName":"Hye","middleName":"Rin","lastName":"Chang","suffix":""},{"id":591040366,"identity":"a7167ae2-f418-4b9f-b465-a21f9babba90","order_by":8,"name":"Guorong Ma","email":"","orcid":"","institution":"University of Southern Mississippi","correspondingAuthor":false,"prefix":"","firstName":"Guorong","middleName":"","lastName":"Ma","suffix":""},{"id":591040367,"identity":"76cfa8de-92dc-4996-8553-117f236b913d","order_by":9,"name":"Xiaodan Gu","email":"","orcid":"https://orcid.org/0000-0002-1123-3673","institution":"The University of Southern Mississippi","correspondingAuthor":false,"prefix":"","firstName":"Xiaodan","middleName":"","lastName":"Gu","suffix":""},{"id":591040368,"identity":"81ed923e-3872-46c9-8824-de914558ddf3","order_by":10,"name":"Tae Il Lee","email":"","orcid":"","institution":"Gachon University","correspondingAuthor":false,"prefix":"","firstName":"Tae","middleName":"Il","lastName":"Lee","suffix":""},{"id":591040369,"identity":"f6c04813-11a8-461a-9bdc-c7a9c2e4f768","order_by":11,"name":"Won Jin Choi","email":"","orcid":"","institution":"Lawrence Livermore National Laboratory","correspondingAuthor":false,"prefix":"","firstName":"Won","middleName":"Jin","lastName":"Choi","suffix":""}],"badges":[],"createdAt":"2025-08-26 02:40:53","currentVersionCode":1,"declarations":"","doi":"10.21203/rs.3.rs-7457973/v1","doiUrl":"https://doi.org/10.21203/rs.3.rs-7457973/v1","draftVersion":[],"editorialEvents":[],"editorialNote":"","failedWorkflow":false,"files":[{"id":102820291,"identity":"78b9f283-faa7-413e-b0ca-051c5a45166d","added_by":"auto","created_at":"2026-02-17 07:22:42","extension":"png","order_by":1,"title":"Figure 1","display":"","copyAsset":false,"role":"figure","size":6755582,"visible":true,"origin":"","legend":"\u003cp\u003e\u003cstrong\u003eMechanically controlled alignment of semiconducting polymer nanofibers in elastomeric composites for stretchable optoelectronics. a,\u003c/strong\u003e Schematic illustration and representative photographs showing how compressive or tensile strain induces alignment of semiconducting polymer (DPPT-TT) nanofibers within an elastomeric (SEBS) matrix. \u003cstrong\u003eb,\u003c/strong\u003e Schematic representation of experimental setup using reflective infrared (IR) imaging via LiDAR to visualize nanofiber alignment. \u003cstrong\u003ec-d,\u003c/strong\u003e Optical images (top) and corresponding reflective IR images (bottom) obtained by LiDAR camera, illustrating the aligned nanofiber film under tensile strain (c) and multilayer Bouligand-structured blend films (d). Scale bars, 1 cm. \u003cstrong\u003ee,\u003c/strong\u003e Atomic force microscopy (AFM) phase images (left) and corresponding orientation maps generated with GTFiber software (right), comparing fiber orientations in spin-coated (unstrained, upper) and 50% compressed (strained, lower) films. Color scales represent fiber orientation distributions. \u003cstrong\u003ef,\u003c/strong\u003e Quantitative two-dimensional order parameter (S\u003csub\u003e2D\u003c/sub\u003e) as a function of compressive strain. Insets display orientation maps of spin-coated (0%, left), 25% (middle), and 50% (right) compressed films. Bottom insets show polarized optical microscopy images of the 50% compressed films observed under cross-polarized conditions at 0° (left) and 45° (right) orientations. White arrows indicate polarizer directions; yellow arrows show fiber alignment directions. Scale bar, 25 µm. \u003cstrong\u003eg,\u003c/strong\u003e UV-visible absorption spectra of a 50% compressed film (left) and corresponding linear dichroic ratios measured at various polarization angles (right). Inset: Schematic of angles between fiber direction and polarizer axis. \u003cstrong\u003eh,\u003c/strong\u003e Grazing-incidence X-ray diffraction (GIXRD) intensity profiles along the Q\u003csub\u003exy\u003c/sub\u003e axis of the 50% compressed film, measured with the incident beam oriented at different angles relative to the fiber alignment. Inset illustrates relative beam and fiber orientations. \u003cstrong\u003ei-j,\u003c/strong\u003e Transfer characteristics (V\u003csub\u003eD\u003c/sub\u003e = -60 V) of transistor devices with channels oriented parallel (i) and perpendicular (j) to the direction of fiber alignment under various degrees of compressive strain. \u003cstrong\u003ek,\u003c/strong\u003e Field-effect mobility and drain current of transistor devices as a function of compressive strain for both parallel (gray) and perpendicular (green) alignment directions (V\u003csub\u003eD\u003c/sub\u003e = -60 V, V\u003csub\u003eG\u003c/sub\u003e = -60 V). \u003cstrong\u003el,\u003c/strong\u003e Durability tests showing field-effect mobility and drain current of transistors fabricated with 50% compressed films after 10,000 cycles of repeated 100% tensile strain applied parallel (top) and perpendicular (bottom) to the transistor channel direction (V\u003csub\u003eD\u003c/sub\u003e = -60 V, on/off currents recorded at V\u003csub\u003eG\u003c/sub\u003e = -60 V and 0 V, respectively).\u003c/p\u003e","description":"","filename":"image1.png","url":"https://assets-eu.researchsquare.com/files/rs-7457973/v1/fc09426870a5f580592aaf31.png"},{"id":102820289,"identity":"23b8e290-b840-484c-bdd6-6efe6246b928","added_by":"auto","created_at":"2026-02-17 07:22:42","extension":"png","order_by":2,"title":"Figure 2","display":"","copyAsset":false,"role":"figure","size":1442047,"visible":true,"origin":"","legend":"\u003cp\u003e\u003cstrong\u003e\u003cbr\u003e\n\u003c/strong\u003e\u003c/p\u003e\n\u003cp\u003e\u003cstrong\u003eChiroptical and electrical characteristics of multilayered Bouligand structures. a,\u003c/strong\u003e Schematic illustration of the fabrication process for strain-induced alignment of nanofibers and subsequent construction of multilayer Bouligand structures. \u003cstrong\u003eb-c,\u003c/strong\u003e Circular dichroism (CD) spectra (b) and corresponding dissymmetry factors (g-factor) of absorbance (c) for left-handed (\u003cem\u003eLH\u003c/em\u003e) and right-handed (\u003cem\u003eRH\u003c/em\u003e) stacked films as a function of increasing number of layers. \u003cstrong\u003ed,\u003c/strong\u003e CD intensity values measured at 850 nm for \u003cem\u003eLH\u003c/em\u003e and \u003cem\u003eRH\u003c/em\u003e stacked films with different layer numbers. \u003cstrong\u003ee,\u003c/strong\u003e Stability of the CD intensity at 850 nm for four-layer \u003cem\u003eLH\u003c/em\u003e and \u003cem\u003eRH\u003c/em\u003e stacked films under various experimental conditions: sample flipping, sample rotation, and varying the angle of incident illumination. \u003cstrong\u003ef,\u003c/strong\u003e On- and off-state currents of Bouligand-structured transistor devices under illumination with circularly polarized light (CPL), plotted against the number of stacked layers (drain voltage, V\u003csub\u003eD\u003c/sub\u003e = -60 V for on-state and V\u003csub\u003eD\u003c/sub\u003e = 10 V for off-state). \u003cstrong\u003eg-h,\u003c/strong\u003e Transfer characteristics of four-layer Bouligand devices under different azimuthal rotation angles for \u003cem\u003eRH\u003c/em\u003e (g) and \u003cem\u003eLH\u003c/em\u003e (h) stacked structures (V\u003csub\u003eD\u003c/sub\u003e = -60 V). \u003cstrong\u003ei,\u003c/strong\u003e Drain current measured at different retarder angles for a four-layer \u003cem\u003eRH\u003c/em\u003e stacked transistor at V\u003csub\u003eD\u003c/sub\u003e = 10 V, highlighting polarization sensitivity. \u003cstrong\u003ej,\u003c/strong\u003e Real-time monitoring of drain current variations in a four-layer \u003cem\u003eRH\u003c/em\u003e stacked transistor as a function of changing retarder angles, demonstrating consistent polarization-dependent electrical responses (V\u003csub\u003eD\u003c/sub\u003e = 10 V).\u003c/p\u003e\n\u003cp\u003e\u003cstrong\u003e\u0026nbsp;\u003c/strong\u003e\u003c/p\u003e","description":"","filename":"image2.png","url":"https://assets-eu.researchsquare.com/files/rs-7457973/v1/decfc9606ec2b58d880bd111.png"},{"id":102963060,"identity":"7b17678c-735a-4b49-b2db-dab193e602c2","added_by":"auto","created_at":"2026-02-19 04:13:04","extension":"png","order_by":3,"title":"Figure 3","display":"","copyAsset":false,"role":"figure","size":316734,"visible":true,"origin":"","legend":"\u003cp\u003e\u003cstrong\u003eMechanical robustness and stable chiroptoelectronic performance of stretchable Bouligand-structured photodetector. a,\u003c/strong\u003e CD spectra of Bouligand-structured multilayer films measured under CPL illumination, demonstrating robust optical responses under significant mechanical strains (50% uniaxial and 30% biaxial stretching). \u003cstrong\u003eb,\u003c/strong\u003e Variations in the dissymmetry factor (g-factor) of photocurrent responses for Bouligand-structured devices under mechanical deformation (50% uniaxial and 30% biaxial strain). \u003cstrong\u003ec-d,\u003c/strong\u003e Photocurrent ratio differences between \u003cem\u003eLH\u003c/em\u003e (c) and \u003cem\u003eRH\u003c/em\u003e (d) four-layer stacked devices under various mechanical strains (uniaxial and biaxial) and incident CPL intensities. \u003cstrong\u003ee,\u003c/strong\u003e Dependence of photocurrent g-factor on incident CPL intensity for four-layer Bouligand-structured devices. \u003cstrong\u003ef-g,\u003c/strong\u003e Real-time drain current measurements demonstrating stable and reproducible photocurrent responses for \u003cem\u003eLH\u003c/em\u003e (top) and \u003cem\u003eRH\u003c/em\u003e (bottom) stacked devices under cyclic CPL illumination and mechanical deformation conditions: f, 50% uniaxial strain, g, 30% biaxial strain (gate voltage, V\u003csub\u003eG\u003c/sub\u003e = 10 V; drain voltage, V\u003csub\u003eD\u003c/sub\u003e = −10 V). \u003cstrong\u003eh,\u003c/strong\u003e Response times of devices under varying mechanical conditions, highlighting the preservation of fast optoelectronic responses under mechanical deformation.\u003c/p\u003e","description":"","filename":"image3.png","url":"https://assets-eu.researchsquare.com/files/rs-7457973/v1/047051a17516c73cedee4300.png"},{"id":102820292,"identity":"e16830e8-d957-43a1-9778-6906005bd104","added_by":"auto","created_at":"2026-02-17 07:22:42","extension":"png","order_by":4,"title":"Figure 4","display":"","copyAsset":false,"role":"figure","size":4627684,"visible":true,"origin":"","legend":"\u003cp\u003e\u003cstrong\u003eEnantiomerically switchable chiral optoelectronic detectors and polarization-encoded logic gates. a,\u003c/strong\u003e Schematic illustration of an enantiomerically switchable circular dichroic detector and photographic image of the fabricated active-matrix transistor array. \u003cstrong\u003eb,\u003c/strong\u003e Representative transfer characteristics of a pristine two-layer stacked transistor within the active-matrix array. \u003cstrong\u003ec,\u003c/strong\u003e CD intensity measured at 850 nm for the switchable devices after repeated mechanical deformation (10 stretching cycles at 25% and 50% tensile strains). \u003cstrong\u003ed,\u003c/strong\u003e Mapping of differences in off-state drain current for a pristine active-matrix array under CPL illumination, illustrating high uniformity across the device. \u003cstrong\u003ee-f,\u003c/strong\u003e Real-time drain current responses at 50% tensile strain, showing distinct and reproducible variations upon changing quarter-wave plate (QWP) angles: e, \u003cem\u003eLH\u003c/em\u003e stacked device strained at 90°, f, \u003cem\u003eRH\u003c/em\u003e stacked device strained at 0°. \u003cstrong\u003eg-h,\u003c/strong\u003e Off-state drain current difference mappings of the active-matrix array under CPL illumination with 50% strain applied at different orientations: g, \u003cem\u003eLH\u003c/em\u003e stacked structure (strain at 0°), h, \u003cem\u003eRH\u003c/em\u003e stacked structure (strain at 90°) (drain voltage, V\u003csub\u003eD\u003c/sub\u003e = -60 V). \u003cstrong\u003ei,\u003c/strong\u003e Real-time photocurrent dissymmetry factor (g-factor) measured for \u003cem\u003eLH\u003c/em\u003e stacked (strained at 0°) and \u003cem\u003eRH\u003c/em\u003e stacked (strained at 90°) devices under cyclic 50% tensile strain. \u003cstrong\u003ej,\u003c/strong\u003e Schematic representation of polarization-sensitive logic gate operations (AND, XNOR) converting optical CPL signals into electrical outputs using mechanically switchable devices. \u003cstrong\u003ek,\u003c/strong\u003e Detailed measurement protocol for dynamic conversion of mechanical strain and CPL illumination into discrete electrical signals. \u003cstrong\u003el,\u003c/strong\u003e Experimental logic gate outputs (drain current responses) demonstrating correct AND and XNOR functionalities under systematically varied input conditions: mechanical strain, CPL illumination intensity, strain orientation, and CPL handedness (V\u003csub\u003eG\u003c/sub\u003e = 10 Vand V\u003csub\u003eD\u003c/sub\u003e = −1 V).\u003c/p\u003e\n\u003cp\u003e\u0026nbsp;\u003c/p\u003e","description":"","filename":"image4.png","url":"https://assets-eu.researchsquare.com/files/rs-7457973/v1/6136ffe63d56342e76a95a1a.png"},{"id":103056516,"identity":"df45df44-7c56-402e-97c3-0328cd7ee570","added_by":"auto","created_at":"2026-02-20 09:13:07","extension":"pdf","order_by":0,"title":"","display":"","copyAsset":false,"role":"manuscript-pdf","size":14691146,"visible":true,"origin":"","legend":"","description":"","filename":"manuscript.pdf","url":"https://assets-eu.researchsquare.com/files/rs-7457973/v1/5240f561-0660-4372-a34f-401c780e6b53.pdf"},{"id":102820296,"identity":"dc8a4576-42fb-4bcf-84cc-cc5d5883fb5c","added_by":"auto","created_at":"2026-02-17 07:22:42","extension":"pdf","order_by":1,"title":"","display":"","copyAsset":false,"role":"supplement","size":5405175,"visible":true,"origin":"","legend":"Supplementary Figures","description":"","filename":"20250826SupplementaryInformation.pdf","url":"https://assets-eu.researchsquare.com/files/rs-7457973/v1/6e61d57825e91c9fdca903c8.pdf"},{"id":102820293,"identity":"a12339d9-a9ce-4182-8218-b2a460915331","added_by":"auto","created_at":"2026-02-17 07:22:42","extension":"mp4","order_by":2,"title":"","display":"","copyAsset":false,"role":"supplement","size":16936127,"visible":true,"origin":"","legend":"Movie S1","description":"","filename":"MovieS1.mp4","url":"https://assets-eu.researchsquare.com/files/rs-7457973/v1/398f9d45ac60d0a4b6e34a17.mp4"},{"id":102820295,"identity":"6cf82092-a142-4849-b096-3a3012996106","added_by":"auto","created_at":"2026-02-17 07:22:42","extension":"mp4","order_by":3,"title":"","display":"","copyAsset":false,"role":"supplement","size":19709540,"visible":true,"origin":"","legend":"Movie S2","description":"","filename":"MovieS2.mp4","url":"https://assets-eu.researchsquare.com/files/rs-7457973/v1/b68e6295a6e0729b709c2c49.mp4"}],"financialInterests":"There is \u003cb\u003eNO\u003c/b\u003e Competing Interest.","formattedTitle":"Dynamically Reconfigurable Polarization in Elastomeric Semiconductors for Stretchable Chiroptoelectronics","fulltext":[{"header":"Introduction","content":"\u003cp\u003eControlling and analyzing the polarization states of light is essential for a wide range of optical applications, including displays, spectroscopy, machine vision, and quantum optics.\u003csup\u003e[1-3]\u003c/sup\u003e For example, liquid crystals have revolutionized display optoelectronic technologies by enabling polarization modulation of anisotropic molecules through electric fields, which control both brightness and color via engineered optical filters, resulting in improved color expression and faster response times. In spectroscopy and photonic devices, photoelastic and acousto-optic modulators play a crucial role in processing polarimetric information.\u003csup\u003e[4]\u003c/sup\u003e They enable coherence and interference between beams, support high repetition rates from a few hundred kilohertz (kHz) to several megahertz (MHz) for signal modulation, and enhance signal-to-noise ratios through lock-in amplification.\u003csup\u003e[5]\u003c/sup\u003e However, most polarization modulators are based on rigid optical crystals or fixed optoelectronic devices, rendering them unsuitable for applications such as stretchable photodetectors and reconfigurable bionic artificial eyes. Moreover, the modulation capability of such optical crystals is inherently limited by the deterministic nature of crystalline birefringence, typically allowing only simple polarization switching, such as from vertical to horizontal or from linear to circular.\u003csup\u003e[6,7]\u003c/sup\u003e Even liquid crystals face intrinsic limitations, as their polarization performance strongly depends on the surface properties of alignment layers and the specific orientation of applied electric fields. Consequently, to realize emerging photonic applications such as biomimetic artificial eyes and deformable optics, it is crucial to develop materials that offer dynamically tunable optical anisotropy and polarization states.\u003csup\u003e[8,9]\u003c/sup\u003e\u003c/p\u003e\n\u003cp\u003eFlexible optoelectronic systems, such as polarization-resolved chiral-responsive devices, require not only optical filters selective to angular momentum but also stretchable photodetectors capable of mechanical deformation.\u003csup\u003e[10]\u003c/sup\u003e Recent studies have pursued enantioselective devices by integrating chiral metasurfaces with various organic and inorganic semiconductors.\u003csup\u003e[11,12]\u003c/sup\u003e Examples include chiral perovskite nanostructures and helicoidal nanoparticles interfaced with transparent conductive metal oxides for circularly polarized light (CPL) detection.\u003csup\u003e[13-16]\u003c/sup\u003e Furthermore, chiral heterostructures incorporating carbon nanotubes have shown promise for CPL-based neuromorphic memory and pattern recognition.\u003csup\u003e[17-19]\u003c/sup\u003e Organic molecules, including helicenes, perylene diimide-fused helicenes, (R)- or (S)-1-phenylethylamine, DPA, fullerene, 1,1\u0026prime;-binaphthyl\u0026ndash;2,2\u0026prime;-diamine, and cellulose nanocrystals, have also been integrated into organic field-effect transistor (OFET) architectures to achieve CPL photodetection.\u003csup\u003e[20-26]\u003c/sup\u003e However, these approaches inherently lack mechanical stretchability, as they predominantly rely on rigid organic crystals or inorganic thin-film architectures. Crucially, they also lack dynamic polarization modulation capabilities, specifically the ability to reversibly reconfigure polarization states. This fundamental limitation significantly constrains their potential use in next-generation technologies, such as biomimetic polarization-resolved artificial eyes, stretchable complementary metal-oxide-semiconductor (CMOS) photodetectors, and soft light detection and ranging (LiDAR) systems for advanced humanoid robotics.\u003csup\u003e[27]\u003c/sup\u003e\u003c/p\u003e\n\u003cp\u003eHere, we present an elastomeric semiconductor composite enabling dynamically reconfigurable polarization and robust mechanical stretchability for chiroptoelectronics. This composite consists of semiconducting polymer nanofibers (DPPT-TT, poly(2,5-bis(2-octyldodecyl)-3,6-di(thiophen-2-yl)diketopyrrolo[3,4-c]pyrrole-1,4-dione-alt-thieno[3,2-b]thiophene) embedded within an elastomeric matrix (SEBS, polystyrene-block-poly(ethylene-ran-butylene)-block-polystyrene), forming a blend film capable of reversible optical polarization encoding via mechanical deformation and electrical field modulation (\u003cstrong\u003eFigure 1\u003c/strong\u003e). This molecularly blended film is optically polarization-writable, electrically field-tunable, and highly stretchable. Furthermore, when stacked, the films exhibit interlayer optical and electronic hybridization while retaining their mechanical stretchability.\u003c/p\u003e\n\u003cp\u003e\u003cstrong\u003eMechanically Programmable Alignment of Semiconducting Polymer Nanofibers for Stretchable Optoelectronics\u003c/strong\u003e\u003c/p\u003e\n\u003cp\u003e\u003cstrong\u003eFigure 1a\u003c/strong\u003e shows a schematic illustration of the alignment mechanism of DPPT-TT polymer nanofibers embedded within an elastomeric SEBS matrix, achieved through controlled compressive strain. The degree of nanofiber alignment is systematically regulated by adjusting the pre-strain level of a poly(dimethylsiloxane) (PDMS) stamp (\u003cstrong\u003eSupplementary Fig. 1\u003c/strong\u003e). \u003cstrong\u003eFigures 1b-c\u003c/strong\u003e and \u003cstrong\u003eMovie S1, S2\u003c/strong\u003e present real-time LiDAR imaging, revealing strain-induced linear polarization in the aligned nanofiber blend films. These optoelectronically integrated films demonstrate pronounced linear dichroism (LD) under uniaxial stretching (\u003cstrong\u003eFig. 1c\u003c/strong\u003e) and exhibit circular dichroism (CD) when configured as multilayered stacks with precisely controlled interlayer twist angles (Bouligand structures, \u003cstrong\u003eFig. 1d\u003c/strong\u003e). Such multilayer Bouligand structures display isotropic reflectance under linearly polarized illumination at a near-infrared wavelength (860 nm), clearly contrasting with the anisotropic response seen in single-layer stretched films. The uniform reflectance across the multilayers indicates a homogeneous distribution of circular polarization within the stacked architecture.\u003c/p\u003e\n\u003cp\u003eThe optical properties of the composite film primarily originate from strain-induced nanofiber alignment. Initially, DPPT-TT nanofibers spontaneously form randomly oriented networks within the SEBS elastomer through nanoconfined phase separation, driven by strong intermolecular \u0026pi;\u0026ndash;\u0026pi; interactions (\u003cstrong\u003eSupplementary Fig. 2\u003c/strong\u003e).\u003csup\u003e\u0026nbsp;[28-30]\u003c/sup\u003e Upon applying compressive strain, these nanofibers uniformly align perpendicular to the strain direction, significantly decreasing inter-fiber spacing, as directly observed by phase-mode atomic force microscopy (AFM) (\u003cstrong\u003eFig. 1e\u003c/strong\u003e and \u003cstrong\u003eSupplementary Figs. 3,4\u003c/strong\u003e). Cross-polarized optical microscopy (inset \u003cstrong\u003eFig. 1f\u003c/strong\u003e, \u003cstrong\u003eSupplementary Fig. 5\u003c/strong\u003e) further confirms uniform nanofiber alignment throughout the films. The degree of alignment, quantified by a two-dimensional order parameter (S\u003csub\u003e2D\u003c/sub\u003e), increases linearly with applied compressive strain (\u003cstrong\u003eFig. 1f\u003c/strong\u003e) and is fully reversible upon strain release, restoring the nanofibers to their original random orientation. Aligned composite films exhibit linear dichroism ratios strongly correlated with S\u003csub\u003e2D\u003c/sub\u003e under compressive strain (\u003cstrong\u003eFig. 1g\u003c/strong\u003e, \u003cstrong\u003eSupplementary Fig. 6\u003c/strong\u003e). Grazing-incidence X-ray diffraction (GIXRD) analyses demonstrate that nanofiber alignment induced by 50% compressive strain correlates directly with preferential molecular orientations in crystalline domains, characterized by prominent (h00) reflections along the Q\u003csub\u003exy\u003c/sub\u003e direction (\u003cstrong\u003eFig. 1h\u003c/strong\u003e, \u003cstrong\u003eSupplementary Fig. 7\u003c/strong\u003e).\u003csup\u003e[31]\u003c/sup\u003e Enhanced diffraction intensities occur when the incident X-ray beam is oriented parallel (0\u0026deg;) to the aligned nanofibers rather than perpendicular (90\u0026deg;), confirming highly oriented crystalline domains (\u003cstrong\u003eSupplementary Fig. 8\u003c/strong\u003e).\u003c/p\u003e\n\u003cp\u003eStrain-induced nanofiber alignment imparts significant anisotropy not only optically but also electrically, as demonstrated in organic field-effect transistors (OFETs) (\u003cstrong\u003eSupplementary Fig. 9\u003c/strong\u003e). OFET channels were defined parallel (∥) or perpendicular (\u0026perp;) to the nanofiber alignment axis (\u003cstrong\u003eFig. 1i,j\u003c/strong\u003e). Compared to the pristine device (randomly oriented DPPT-TT nanofibers, \u0026mu;\u003csub\u003eeff\u003c/sub\u003e = 0.40 cm\u0026sup2;/V\u0026middot;s), devices with nanofibers aligned at 50% strain parallel to the charge transport direction exhibited more than twofold enhanced field-effect mobility (0.9 cm\u0026sup2;/V\u0026middot;s). Conversely, mobility decreased approximately by half (0.20 cm\u0026sup2;/V\u0026middot;s) in the perpendicular orientation, while maintaining consistently low leakage currents (~10\u003csup\u003e-10\u003c/sup\u003e A) and high on/off current ratios (\u0026gt;10\u003csup\u003e4\u003c/sup\u003e) (\u003cstrong\u003eFig. 1k\u003c/strong\u003e, \u003cstrong\u003eSupporting Note 4\u003c/strong\u003e, \u003cstrong\u003eSupplementary Figs. 13-16\u003c/strong\u003e). These differences primarily stem from alignment-induced formation of efficient charge percolation pathways along the current direction, as further supported by reductions in activation energy (E\u003csub\u003eA\u003c/sub\u003e), Urbach energy (E\u003csub\u003eU\u003c/sub\u003e), and contact resistance (R\u003csub\u003eC\u003c/sub\u003e) (\u003cstrong\u003eSupporting Note 5\u003c/strong\u003e). Moreover, our devices demonstrate outstanding mechanical durability, retaining stable mobility, drain current, and optical anisotropy even after 10,000 cycles of repeated stretching at 100% tensile strain (\u003cstrong\u003eFig. 1l\u003c/strong\u003e, \u003cstrong\u003eSupplementary Figs. 24-26\u003c/strong\u003e).\u003c/p\u003e\n\u003cp\u003e\u003cstrong\u003eMultilayer Bouligand Structures for Chiral Optoelectronic Detection and Polarization-Encoding\u003c/strong\u003e\u0026nbsp;\u003c/p\u003e\n\u003cp\u003eExpanding on our findings from single-layer films, we explored multilayered structures composed of individually aligned blend films stacked at precise twist angles. These multilayers exhibit emergent chiral optical and electrical characteristics originating explicitly from controlled interlayer twist angles rather than cumulative linear polarization. To investigate these chiroptical properties, we fabricated OFETs incorporating helically stacked blend films arranged into Bouligand structures, with each successive layer rotated by 45\u0026deg; relative to the underlying layer (\u003cstrong\u003eFig. 2a\u003c/strong\u003e). Each aligned film (80 nm thickness) was prepared by transferring a nanofiber-aligned polymer layer from a pre-strained (100% tensile) PDMS stamp onto an elastomeric SEBS substrate (0.2 mm thick). Multilayer structures (2-4 layers) were constructed sequentially with precisely defined twist orientations to left-handed (\u003cem\u003eLH\u003c/em\u003e) and right-handed (\u003cem\u003eRH\u003c/em\u003e) directions to form robust, electrically interconnected assemblies.\u0026nbsp;\u003c/p\u003e\n\u003cp\u003eThe helically stacked films showed distinct circular dichroism (CD) peaks near 750 nm and 850 nm, corresponding respectively to H- and J-type molecular aggregations within DPPT-TT semiconductors (\u003cstrong\u003eFig. 2b\u003c/strong\u003e; \u003cstrong\u003eSupplementary Fig. 27\u003c/strong\u003e).\u003csup\u003e[32-34]\u003c/sup\u003e Single-layer films exhibited negligible CD signals, whereas bilayer stacks displayed pronounced mirror-symmetric CD absorption bands near 850 nm, indicating hybridized chiral electronic states. As layer number increased, CD intensity progressively amplified to 1,500 mdeg, corresponding to a substantial dissymmetry factor of absorbance (g-factor \u0026asymp; 0.1), defined as \u0026nbsp;), where\u0026nbsp;\u0026nbsp;\u0026nbsp;and\u0026nbsp;\u0026nbsp;\u0026nbsp;represent the absorption under left (\u003cem\u003eL\u003c/em\u003e-) and right (\u003cem\u003eR\u003c/em\u003e-) CPL, respectively (\u003cstrong\u003eFig. 2c\u003c/strong\u003e). A slight redshift of the main absorption peak to ~870 nm further confirmed enhanced \u0026pi;-conjugation and exciton coupling across the layers.\u003c/p\u003e\n\u003cp\u003eNeither pure SEBS nor neat DPPT-TT films exhibited intrinsic chiroptical activity, verifying that the observed chirality emerged solely from the ordered alignment and interlayer hybridization of nanofibers rather than inherent molecular chirality (\u003cstrong\u003eSupplementary Figs. 28,29\u003c/strong\u003e).\u0026nbsp;Multilayer structures and large-scale solid samples often exhibit \u003cem\u003eapparent\u003c/em\u003e CD behavior due to compositional optical effects arising from interactions between layers with distinctly different optical properties, such as dichroism and birefringence.\u003csup\u003e[35]\u003c/sup\u003e Angular-dependent CD measurements showed negligible variation upon azimuthal angle rotation and reversed illumination direction, as confirmed by Mueller matrix symmetry conditions (M\u003csub\u003e03\u003c/sub\u003e = M\u003csub\u003e30\u003c/sub\u003e), strongly supporting genuine structural chirality from the stacked architecture (\u003cstrong\u003eFig. 2d,e\u0026nbsp;\u003c/strong\u003eand\u003cstrong\u003e\u0026nbsp;Supplementary Figs. 30\u0026ndash;32\u003c/strong\u003e).\u003c/p\u003e\n\u003cp\u003eOur multilayered films demonstrate chiral, gate-tunable transistor functionality achievable only when the nanofibers exhibit both strong optical anisotropy and efficient three-dimensional charge-transport pathways, characteristics not attainable with conventional chiral materials such as linear optically active chromophores, Langmuir-Blodgett films, or chiral nanoparticle assemblies.\u003csup\u003e[36]\u003c/sup\u003e Strong exciton coupling involving \u0026pi;-\u0026pi; transitions and charge-transfer states results in pronounced polarization-dependent photocurrents under CPL illumination. Stacked chiroptoelectronic transistors displayed significant stereoselective enhancement of off-state current upon illumination with co-polarized CPL, attributed to enhanced photocarrier generation in the transistor channel (\u003cstrong\u003eFig. 2f\u003c/strong\u003e and \u003cstrong\u003eSupplementary Fig. 33\u003c/strong\u003e). Devices comprising up to four stacked layers consistently exhibited clear trends in on/off currents under \u003cem\u003eL-\u003c/em\u003e and \u003cem\u003eR-\u003c/em\u003eCPL illumination, maintaining over 10⁴ on/off current ratios despite substantial modulation of the off-state current (\u003cstrong\u003eFig. 2f\u003c/strong\u003e). Additionally, four-layer Bouligand structures showed isotropic optical responses, substantially minimizing azimuthal-angle dependence of transistor characteristics (\u003cstrong\u003eFig. 2g,h\u003c/strong\u003e).\u003c/p\u003e\n\u003cp\u003eBeyond fundamental CPL detection, the multilayered Bouligand films provided helicity-selective electronic outputs enabling advanced polarization-based digital functionalities. Unlike conventional CPL photodetectors limited to binary polarization detection (\u003cem\u003eL-\u003c/em\u003e or \u003cem\u003eR-\u003c/em\u003eCP), our devices continuously differentiate polarization states ranging from linear to elliptical to circular, highlighting their applicability for real-time polarization-resolved computing and secure optical communication. Moreover, four-layer stacked films demonstrated direct extraction of retarder angles by monitoring transistor drain current at the off-state (V\u003csub\u003eG\u003c/sub\u003e = 10 V), under continuously varying (\u003cstrong\u003eFig. 2i\u003c/strong\u003e) and digitally randomized polarization inputs (\u003cstrong\u003eFig. 2j\u003c/strong\u003e and \u003cstrong\u003eSupplementary Fig. 34\u003c/strong\u003e). This capability strongly suggests potential applications in advanced data transmission and secure optical encryption, analogous to emerging infrared-based optical communication technologies such as Li-Fi.\u003c/p\u003e\n\u003cp\u003e\u003cstrong\u003eMechanically Robust Multilayer Bouligand-Structured Semiconducting Elastomers for Stretchable Chiral Photodetection\u003c/strong\u003e\u0026nbsp;\u003c/p\u003e\n\u003cp\u003eA fundamental advantage of elastomeric semiconductor films is their inherent softness and elasticity, suited for emerging stretchable chiroptoelectronic applications. Unlike conventional rigid optical crystals, our elastomeric composite closely matches the elastic modulus of human skin, demonstrating exceptional mechanical resilience and flexibility. To quantitatively assess this capability, we investigated \u003cem\u003eLH\u003c/em\u003e and \u003cem\u003eRH\u003c/em\u003e multilayer (4-layer) Bouligand-structured OFETs under substantial mechanical deformation (\u003cstrong\u003eFig. 3\u003c/strong\u003e and \u003cstrong\u003eSupplementary Figs. 35,36\u003c/strong\u003e). The key optical and electrical properties remained robust under both uniaxial (up to 50%) and biaxial (up to 30%) tensile strains. Even at 30% biaxial strain, differences in the off-state current responses to \u003cem\u003eL-\u003c/em\u003e and \u003cem\u003eR-\u003c/em\u003eCPL were nearly identical to those in unstrained devices, confirming reliable chirality-selective detection under complex mechanical environments (\u003cstrong\u003eSupplementary Figs. 37-41\u003c/strong\u003e).\u003c/p\u003e\n\u003cp\u003eThe CD measurements further verified the mechanical stability of chiral optical properties. Under 50% uniaxial strain, CD intensity decreased modestly (~28%), accompanied by a 99 nm blue shift, while under 30% biaxial strain, CD intensity decreased by approximately 22% with a 32 nm blue shift (\u003cstrong\u003eFig. 3a\u003c/strong\u003e and \u003cstrong\u003eSupplementary Figs. 42-44\u003c/strong\u003e). Despite mechanical deformation, the resilience of CD spectra underscores the critical influence of precisely controlled interlayer twist angles in preserving chiroptical responses. These mechanical perturbations resulted only in minor (~10% for \u003cem\u003eLH\u003c/em\u003e and ~15% for \u003cem\u003eRH\u003c/em\u003e configurations) reductions in the dissymmetry factor (g\u003csub\u003eph\u003c/sub\u003e), further validating the mechanical and optical robustness of the composites (\u003cstrong\u003eFig. 3b\u003c/strong\u003e and \u003cstrong\u003eSupplementary Fig. 45\u003c/strong\u003e).\u003c/p\u003e\n\u003cp\u003eThe primary performance metric of the elastic Bouligand-structured semiconductor is the magnitude of photocurrent differences generated by \u003cem\u003eL-\u003c/em\u003e and \u003cem\u003eR-\u003c/em\u003eCPL illumination under identical intensities. To quantitatively evaluate sensor performance, we analyzed the sensitivity and linear dynamic range (LDR) by monitoring photocurrent differences as a function of incident light intensity, both before and after mechanical deformation (\u003cstrong\u003eFig. 3c,d\u003c/strong\u003e and \u003cstrong\u003eSupplementary Figs. 46,47\u003c/strong\u003e). The pristine devices showed a linear dynamic range of 0.645-1.504 mW/cm\u0026sup2; and sensitivity of approximately 27-31 cm\u0026sup2;/mW. These key metrics remained largely unaffected by significant uniaxial (50%) and biaxial (30%) tensile strains, demonstrating exceptional mechanical reliability and stable performance (\u003cstrong\u003eFig. 3e\u003c/strong\u003e and \u003cstrong\u003eSupplementary Table 2\u003c/strong\u003e).\u003c/p\u003e\n\u003cp\u003eTo gain further insight into dynamic optoelectronic stability, we investigated the time-resolved photocurrent responses of the OFET devices. Under cyclic illumination with alternating \u003cem\u003eL-\u003c/em\u003e and \u003cem\u003eR-\u003c/em\u003eCPL, pristine devices consistently exhibited distinct and stable photocurrent states corresponding to co- and cross-polarized conditions, respectively. The response and recovery times of both \u003cem\u003eRH\u003c/em\u003e and \u003cem\u003eLH\u003c/em\u003e configurations were measured to be approximately 2.01 \u0026plusmn; 0.2 s and 1.08 \u0026plusmn; 0.3 s, respectively (\u003cstrong\u003eSupplementary Figs. 48,49\u003c/strong\u003e). These rapid response characteristics remained stable under significant mechanical strain conditions (50% uniaxial and 30% biaxial), demonstrating exceptional dynamic robustness (\u003cstrong\u003eFig. 3f-h\u003c/strong\u003e). Collectively, these results confirm that the controlled interlayer twist angle predominantly governs the enantioselective optical response of the device, exhibiting superior robustness over uniformly applied mechanical deformation.\u003c/p\u003e\n\u003cp\u003e\u003cstrong\u003eMechanically Reconfigurable Chiral Optoelectronics\u003c/strong\u003e\u003c/p\u003e\n\u003cp\u003eA distinctive feature of this elastomeric semiconductor composite is its distinctive ability to dynamically and reversibly program optical polarization states through mechanical strain, analogous to data writing and erasing processes in electronic memory devices, while simultaneously operating as transistors. Additionally, unlike mechanically reconfigurable films comprising dye or liquid crystal blends with nanomaterials, our material inherently integrates transistor functionality.\u0026nbsp;\u003c/p\u003e\n\u003cp\u003eThis versatile capability is realized using a minimal bilayer architecture, wherein the top layer initially consists of randomly oriented nanofibers, while the bottom layer is pre-aligned through 50% compressive strain at a 45\u0026deg; orientation relative to the substrate (\u003cstrong\u003eFig. 4a\u003c/strong\u003e). Upon applying 50% tensile strain, nanofibers in the top isotropic layer directionally align, while the pre-aligned bottom layer remains effectively stable (\u003cstrong\u003eSupplementary Fig. 50\u003c/strong\u003e). Leveraging this design, we fabricated a 5\u0026times;5 active-matrix transistor array capable of selectively detecting \u003cem\u003eL-\u003c/em\u003e and \u003cem\u003eR-\u003c/em\u003eCPL by simply adjusting the direction of applied mechanical strain (\u003cstrong\u003eFig. 4b\u003c/strong\u003e and \u003cstrong\u003eSupplementary Fig. 51\u003c/strong\u003e). All pixel transistors exhibited highly uniform, hysteresis-free electrical responses to CPL illumination, preserving stable performance even after repeated uniaxial stretching cycles up to 50% strain (\u003cstrong\u003eSupplementary Fig. 52\u003c/strong\u003e).\u003c/p\u003e\n\u003cp\u003eThe CD measurements demonstrated stable optical characteristics, consistently maintaining ~500 mdeg intensity under repeated 25% tensile strain and significantly increasing to approximately ~700 mdeg under 50% tensile strain (\u003cstrong\u003eFig. 4c\u003c/strong\u003e; \u003cstrong\u003eSupplementary Figs. 53,54\u003c/strong\u003e). This enhancement originates from increased molecular ordering and improved intermolecular interactions induced by moderate mechanical strain. Correspondingly, the optoelectronic characteristics exhibited remarkable robustness, comparable to multilayer Bouligand structures. In an unstrained state, transistor arrays showed highly uniform off-current ratios (I\u003csub\u003eLCPL\u003c/sub\u003e/I\u003csub\u003eRCPL\u003c/sub\u003e: 1.05; \u003cstrong\u003eFig. 4d\u003c/strong\u003e). Under mechanical deformation (50% uniaxial strain), the devices demonstrated precise discrimination among linear, elliptical, and circular polarization states, consistently generating reproducible photocurrent signals (\u003cstrong\u003eFig. 4e,f\u003c/strong\u003e and \u003cstrong\u003eSupplementary Fig. 55\u003c/strong\u003e). Illumination with CPL matching the mechanically induced chirality significantly enhanced the off-state current, yielding nearly an order-of-magnitude increase compared to illumination with opposite-handed CPL (\u003cstrong\u003eFig. 4g,h\u003c/strong\u003e and \u003cstrong\u003eSupplementary Figs. 56-58\u003c/strong\u003e). Importantly, the photocurrent asymmetry, quantified by the dissymmetry factor (g\u003csub\u003eph\u003c/sub\u003e = 0.65), remained exceptionally stable through multiple 50% stretching cycles (\u003cstrong\u003eFig. 4i\u003c/strong\u003e).\u003c/p\u003e\n\u003cp\u003eCapitalizing on the demonstrated mechanically tunable CPL sensitivity, we further implemented a polarization-sensitive optoelectronic logic gate capable of fundamental logic operations (AND, XNOR) modulated by mechanical deformation and CPL illumination (\u003cstrong\u003eFig. 4j\u003c/strong\u003e and \u003cstrong\u003eSupplementary Fig. 59\u003c/strong\u003e). Our experimental protocol systematically translated mechanical and optical stimuli into discrete electrical outputs through three sequential stages (\u003cstrong\u003eFig. 4k\u003c/strong\u003e). Initially (Stage 1), baseline off-state currents were established in the unstrained, dark condition. Subsequently (Stage 2), intrinsic polarization sensitivity was evaluated under sequential L- and R-CPL illumination without applied strain. In the final step (Stage 3), applying 50% tensile strain either parallel or perpendicular to the substrate axis set distinct polarization-sensitive axes (+45\u0026deg; or -45\u0026deg;), allowing selective and reproducible photocurrent responses to CPL illumination.\u003c/p\u003e\n\u003cp\u003eExplicit logic gate demonstration involved defining binary inputs based on controlled parameters: mechanical strain (logic \u0026apos;0\u0026apos; = 0%, logic \u0026apos;1\u0026apos; = 50% strain) and CPL illumination intensity (logic \u0026apos;0\u0026apos; = dark, logic \u0026apos;1\u0026apos; = 1.6 mW/cm\u0026sup2;). The AND gate exhibited high photocurrent output (\u0026apos;1\u0026apos;) only with simultaneous strain and illumination inputs. For the XNOR gate, binary inputs included strain direction (90\u0026deg; as \u0026apos;0\u0026apos;, 0\u0026deg; as \u0026apos;1\u0026apos;) relative to pre-aligned layers and CPL handedness (LCP as \u0026apos;0\u0026apos;, RCP as \u0026apos;1\u0026apos;), producing high output only when inputs matched. All logic input combinations generated accurate and reproducible outputs (\u003cstrong\u003eFig. 4l\u003c/strong\u003e and \u003cstrong\u003eSupplementary Table 3\u003c/strong\u003e). An elastomeric semiconductor platform capable of robustly and reversibly encoding chiral optical states, while simultaneously maintaining stable transistor functionality under extensive mechanical deformation. This integrated system-level approach unlocks unprecedented opportunities in stretchable chiroptoelectronics.\u003c/p\u003e"},{"header":"Methods","content":"\u003cp\u003e\u003cstrong\u003eMaterials:\u0026nbsp;\u003c/strong\u003e\u003c/p\u003e\n\u003cp\u003ePoly(2,5-bis(2-octyldodecyl)-3,6-di(thiophen-2-yl)diketopyrrolo[3,4-c]pyrrole-1,4-dione-alt-thieno[3,2-b]thiophen) (DPPT-TT) (Derthon, M\u003csub\u003ew\u003c/sub\u003e/M\u003csub\u003en\u003c/sub\u003e = 100k/42k) polymer was traded by Derthon. Polystyrene-block-poly(ethylene-ranbutylene)-block-polystyrene (SEBS) was purchased from Asahi Kasei company. Poly(-dimethylsiloxane) (PDMS, Sylgard 184) and its cross-linker were supported by Dow Corning. The PDMS was cured with a ratio of 10:1 (base/cross-linker, w/w) at 65 \u0026deg;C overnight for the transfer printing stamp. Ag (silver, 99.99%, 3\u0026ndash;5 mm granule) was purchased from SY SCIENCE. The Trichloro(octadecyl)silane (OTS) solution and diiodomethane were purchased by Sigma Aldrich. Anhydrous chlorobenzene, chloroform, and toluene were purchased by Sigma Aldrich. All chemicals and materials were used without any purification.\u003c/p\u003e\n\u003cp\u003e\u003cstrong\u003eDevice fabrications and characterizations\u003c/strong\u003e\u003c/p\u003e\n\u003cp\u003e\u003cstrong\u003eFully stretchable transistors:\u0026nbsp;\u003c/strong\u003e\u003c/p\u003e\n\u003cp\u003e\u003cstrong\u003eThin film preparation.\u003c/strong\u003e The semiconductor solution was prepared by dissolving DPPT-TT (0.21 wt%) and SEBS H1062 (S/EB weight ratio of 18/82, 0.49 wt%) with a total of 0.7 wt%, in anhydrous chlorobenzene at 120 \u0026deg;C for 4 h. The solution was spun on an OTS-treated SiO\u003csub\u003e2\u003c/sub\u003e/Si wafer at 1000 rpm for 1 min after filtration with a PTFE-D (0.2 \u0026mu;m) filter (film thickness: 80 nm). The semiconducting film was then annealed at 180 \u0026deg;C for 1 hour. All processes were carried out under an N\u003csub\u003e2\u003c/sub\u003e atmosphere in a glove box with extremely low levels of moisture (H\u003csub\u003e2\u003c/sub\u003eO \u0026lt; 0.01 parts per million (ppm)) and oxygen (O\u003csub\u003e2\u003c/sub\u003e \u0026lt; 0.01 ppm). The SEBS H1052 dielectric solution (S/EB weight ratio of 20/80, 60 mg/mL in toluene) was dissolved at 70 \u003csup\u003eo\u003c/sup\u003eC for 4 h in ambient condition, then, was spun at 1000 rpm for 1 min (film thickness: 1200 nm) on OTS-treated SiO\u003csub\u003e2\u003c/sub\u003e without any heat treatment.\u003c/p\u003e\n\u003cp\u003e\u003cstrong\u003eFully stretchable transistor preparation.\u003c/strong\u003e The elastomer substrates were prepared by casting SEBS H1062 (100 mg/ml in toluene) onto glass slides to form elastic films with the approximate thickness around 0.2 mm. Ag gate electrode (50 nm thick) was thermally evaporated onto the SEBS substrate at a speed of 0.2 nm/s under high vacuum conditions (below 6.0 \u0026times; 10\u003csup\u003e\u0026minus;6\u003c/sup\u003e torr). SEBS H1052 dielectric and semiconducting film on OTS-treated SiO\u003csub\u003e2\u003c/sub\u003e were sequentially transferred onto the gate electrode. Finally, the 50 nm-thick source/drain electrodes were evaporated at a rate of 0.2 nm/s using a thermal evaporator one to form the top contact/bottom gate field-effect-transistor structure. The channel length and width were 1000 and 150 \u0026mu;m, respectively. The semiconducting layers were stacked in clockwise direction and counterclockwise direction with 45-degree to the beneath layer in each stacked layer to achieve Bouligand structure.\u0026nbsp;\u003c/p\u003e\n\u003cp\u003e\u003cstrong\u003eActive-matrix transistor array for logic gate function.\u003c/strong\u003e All the procedures were identical to the fabrication process of fully stretchable transistors, except for the dielectric film. The dielectric layer with a different concentration (75 mg/ml in toluene, 1.8 \u0026mu;m thick) was used and spin-coated at 1000 rpm for 1 min to achieve a thicker dielectric film to reduce leakage current.\u003c/p\u003e\n\u003cp\u003e\u003cstrong\u003eBouligand structure for optical measurements\u003c/strong\u003e. The semiconducting layers were transferred and stacked in clockwise direction and counterclockwise direction with 45-degree twist angles to the beneath layer on SEBS substrate. \u0026nbsp;\u003c/p\u003e\n\u003cp\u003e\u003cstrong\u003eCharacterization\u003c/strong\u003e\u003c/p\u003e\n\u003cp\u003eFor stabilization of the devices, all devices were aged overnight in an auto-dry desiccator. The electrical characteristics of devices were measured using probe station connected with KEITHLEY 4200 and direct current generator (OWON, P4305) under ambient condition. To maximize photo-response current, a laser at 830 nm was selected with a power density of 1.6 mW/cm\u0026sup2; and a beam diameter of 0.2 mm, corresponding to the peak where CD absorption is maximized (Fig. 2b). \u0026nbsp;The capacitances of dielectric were measured using probe station connected with LCR meter (Keysight 4274A). The UV-Vis-Nir and polarized UV-Vis-Nir spectrums were obtained with spectrophotometer (JASCO, V-770). The surface structures and current images were obtained with atomic force microscopy (AFM; Bruker MultiMode 8-HR) under ambient condition. The optical images and polarized optical images obtained with optical microscope (OM; Leica DM4 M). The thickness of the films was obtained with an ellipsometer (WONWOO STRC-2000). Grazing incidence X-ray diffraction (GIXD) patterns of semiconducting thin films were performed on a laboratory beamline system (Xenocs Inc. Xeuss 2.0) with an X‐ray wavelength of 1.54 \u0026Aring; and sample to detector distance of 15 cm. Samples were kept under vacuum to minimize air scattering. The surface energy and contact angle were obtained by PHOENIX-MT(T). The CD spectra was measured using JASCO-815 CD spectrometer with NIR detector from 300nm - 900nm, 0.5msec, 1s D.I.T. and from 700nm - 1100nm, 0.5msec, 1s D.I.T.\u003c/p\u003e"},{"header":"Declarations","content":"\u003cp\u003e\u003cstrong\u003eAcknowledgments\u003c/strong\u003e\u003c/p\u003e\n\u003cp\u003eThis research was supported by Basic Science Research Program through the National Research Foundation of Korea (NRF) funded by the Ministry of Education (RS-2021-NR061555 and RS-2020-NR049601), GRRC program of Gyeonggi province (GRRCKYUNGHEE2023-B03), the Korea Institute for Advanced of Technology (KIAT) and the Ministry of Trade, Industry \u0026amp; Energy (MOTIE) of the Republic of Korea (RS-2024-00434908 and RS-2025-25435993), and the auspices of the U.S. Department of Energy by Lawrence Livermore National Laboratory under Contract DE-AC52-07NA27344. W.J.C. gratefully acknowledge the LLNL LDRD Program for funding support of this project under No.22-ERD-056. X.G. and G.M. thanks NSF for supporting the morphology characterizations performed in this work under award number CHE-2304969.\u003c/p\u003e\n\u003cp\u003e\u003cstrong\u003eAuthor contributions\u003c/strong\u003e\u003c/p\u003e\n\u003cp\u003eN.T.P.V. and J.Y.O. conceived the study and N.T.P.V., W.C., T.I.L., and J.Y.O. designed the experiments. N.T.P.V. conducted all experiments. N.T.P.V., T.U.N., M.W.J., K.H.J., T.A.N., S.H.P., H.R.C., G.M., X.G., T.I.L., W.C., and J.Y.O. analyzed and discussed the data. N.T.P.V., T.I.L., W.C., and J.Y.O. wrote the manuscript.\u003c/p\u003e\n\u003cp\u003e\u003cstrong\u003eCompeting interests\u003c/strong\u003e\u003c/p\u003e\n\u003cp\u003eAuthors declare that they have no competing interests.\u003c/p\u003e\n\u003cp\u003e\u003cstrong\u003eData availability\u003c/strong\u003e\u003c/p\u003e\n\u003cp\u003eData are available on request. Correspondence and requests for materials should be addressed to T.I.L., W.J.C., and J.Y.O.\u0026nbsp;\u003c/p\u003e\n\u003cp\u003e\u003cstrong\u003eSupplementary information\u003c/strong\u003e\u0026nbsp;\u003c/p\u003e\n\u003cp\u003eThe online version contains supplementary material available at https://doi.org/##.####\u003c/p\u003e"},{"header":"References","content":"\u003col\u003e\n \u003cli\u003eJan, C. M., Lee, Y. H., Wu, K. C. \u0026amp; Lee, C. K. Integrating fault tolerance algorithm and circularly polarized ellipsometer for point-of-care applications. \u003cem\u003eOpt. Express\u003c/em\u003e \u003cstrong\u003e19\u003c/strong\u003e, 5431\u0026ndash;5441 (2011).\u003c/li\u003e\n \u003cli\u003eSherson, J. F. et al. Quantum teleportation between light and matter. \u003cem\u003eNature\u003c/em\u003e \u003cstrong\u003e443\u003c/strong\u003e, 557\u0026ndash;560 (2006).\u003c/li\u003e\n \u003cli\u003eWagenknecht, C. et al. 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Phys. Chem. B\u003c/em\u003e \u003cstrong\u003e107\u003c/strong\u003e, 2565\u0026ndash;2569 (2003).\u003c/li\u003e\n\u003c/ol\u003e"}],"fulltextSource":"","fullText":"","funders":[],"hasAdminPriorityOnWorkflow":false,"hasManuscriptDocX":true,"hasOptedInToPreprint":true,"hasPassedJournalQc":"","hasAnyPriority":true,"hideJournal":false,"highlight":"","institution":"","isAcceptedByJournal":false,"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-7457973/v1","lastPublishedDoiUrl":"https://doi.org/10.21203/rs.3.rs-7457973/v1","license":{"name":"CC BY 4.0","url":"https://creativecommons.org/licenses/by/4.0/"},"manuscriptAbstract":"Stretchable optoelectronics capable of dynamically controlling and detecting circularly polarized light offer transformative potential for wearable optoelectronic computing, biomimetic sensing, and photonic communication. However, conventional polarization-sensitive materials based on rigid birefringent optical crystals or chiral organic compounds inherently lack mechanical adaptability and reversible polarization tunability. Here, we introduce a mechanically robust, stretchable composite based on alignment-controllable semiconducting polymer nanofibers embedded in an elastomer matrix, which exhibits dynamically tunable optical activity through mechanical deformation and/or angular layer assembly. By stacking individual layers at controlled twist angles, we achieve highly sensitive chiroptical detection in the near-infrared range even under mechanical deformation (up to 50 % uniaxial and 30 % biaxial strain) for stretchable optoelectronics. Furthermore, our devices demonstrate reliable optoelectrical performance with high reproducibility under repeated stretching cycling, maintaining polarization-selective transistor functionality and enabling mechanically programmable optical logic gates (AND, XNOR). Our findings establish a transformative paradigm for mechanically adaptive chiroptoelectronics, enabling skin-integrated photonic sensing and computing.","manuscriptTitle":"Dynamically Reconfigurable Polarization in Elastomeric Semiconductors for Stretchable Chiroptoelectronics","msid":"","msnumber":"","nonDraftVersions":[{"code":1,"date":"2026-02-17 07:22:37","doi":"10.21203/rs.3.rs-7457973/v1","editorialEvents":[],"status":"published","journal":{"display":true,"email":"[email protected]","identity":"nature-photonics","isNatureJournal":true,"hasQc":false,"allowDirectSubmit":false,"externalIdentity":"nphoton","sideBox":"Learn more about [Nature Photonics](https://www.nature.com/nphoton/)","snPcode":"41566","submissionUrl":"https://mts-nphot.nature.com/cgi-bin/main.plex","title":"Nature Photonics","twitterHandle":"","acdcEnabled":true,"dfaEnabled":true,"editorialSystem":"ejp","reportingPortfolio":"Nature Research","inReviewEnabled":true,"inReviewRevisionsEnabled":false}}],"origin":"","ownerIdentity":"227208f5-d1ca-4a8b-a116-b5e0268ec6bd","owner":[],"postedDate":"February 17th, 2026","published":true,"recentEditorialEvents":[],"rejectedJournal":[],"revision":"","amendment":"","status":"under-review","subjectAreas":[{"id":62900603,"name":"Physical sciences/Optics and photonics/Optical materials and structures/Nanowires"},{"id":62900604,"name":"Physical sciences/Materials science/Materials for devices/Sensors and biosensors"},{"id":62900605,"name":"Physical sciences/Nanoscience and technology/Nanoscale materials/Nanowires"},{"id":62900606,"name":"Physical sciences/Physics/Electronics, photonics and device physics/Electronic and spintronic devices"}],"tags":[],"updatedAt":"2026-02-17T07:22:37+00:00","versionOfRecord":[],"versionCreatedAt":"2026-02-17 07:22:37","video":"","vorDoi":"","vorDoiUrl":"","workflowStages":[]},"version":"v1","identity":"rs-7457973","journalConfig":"researchsquare"},"__N_SSP":true},"page":"/article/[identity]/[[...version]]","query":{"redirect":"/article/rs-7457973","identity":"rs-7457973","version":["v1"]},"buildId":"XKTyCvWXoU3ODBz1xrDgd","isFallback":false,"isExperimentalCompile":false,"dynamicIds":[84888],"gssp":true,"scriptLoader":[]}