Multicolor Emission from Ultraviolet GaN-based Photonic Quasicrystal Nanopyramid Structure with Semipolar InxGa1-xN/GaN Multiple Quantum Wells

Multicolor Emission from Ultraviolet GaN-based Photonic Quasicrystal Nanopyramid Structure with Semipolar InxGa1-xN/GaN Multiple Quantum Wells | 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 Research Article Multicolor Emission from Ultraviolet GaN-based Photonic Quasicrystal Nanopyramid Structure with Semipolar In x Ga 1-x N/GaN Multiple Quantum Wells Cheng-Chang Chen, Hsiang-Ting Lin, Shih-Pang Chang, Hao-Chung Kuo, and 4 more This is a preprint; it has not been peer reviewed by a journal. https://doi.org/ 10.21203/rs.3.rs-320128/v1 This work is licensed under a CC BY 4.0 License Status: Under Review Version 1 posted 5 You are reading this latest preprint version Abstract In this study, we demonstrated large-area high quality multi-color emission from the 12-fold symmetric GaN photonic quasicrystal nanorod device which was fabricated using the nanoimprint lithography technology and multiple quantum wells regrowth procedure. High-efficiency blue and green color emission wavelengths of 460 and 520 nm from the regrown In x Ga 1−x N/GaN multiple quantum wells were observed under optical pumping conditions. To confirm the strongly coupling between the quantum well emissions and the photonic crystal band-edge resonant modes, the finite-element method (FEM) was applied to perform a simulation of the 12-fold symmetry photonic quasicrystal lattices. Nanoscience GaN GaN-based LEDs Photonic quasicrystal multicolor emission Finite-element method Figures Figure 1 Figure 2 Figure 3 Figure 4 Figure 5 Main Text The potential applications of GaN-based materials have recently attracted attention because of their large direct band gap and their potential for use in optoelectronic devices, including light emitting diodes (LEDs)[1-3] and laser diodes (LDs).[4-5] GaN-based LEDs have been applied in traffic signals, display backlights,[6-8] solid-state lighting,[9,10] biosensors,[11] and optogenetics.[12] A potential applications for GaN-based LEDs would be in the development of phosphor-free white LEDs, including multichip white LEDs, monolithic LEDs, and color-conversion white LEDs.[13,14] Blue LD can serve as the light source for high-density data storage in a Blu-ray Disc (BD), which is a popular data storage tool. Promoting and increasing the efficiency of the light source is imperative because of its multitude of potential applications. GaN-based nanorods possess low dislocation, low internal field, and high light extraction efficiency, which are the factors intrinsic in improving photoluminescence (PL) intensity.[15,16] Various approaches have been employed to increase the light extraction efficiency for III-nitride LEDs, such as rough surfaces,[17-20] sapphire microlenses,[21] oblique mesa sidewalls,[22] nanopyramids,[23] graded refractive index materials,[24] self-assembled lithography patterning,[25] colloidal-based microlens arrays,[26,27] and photonic crystals.[28–31] Photonic crystals have been reported in quasicrystal or defective two-dimensional (2D) grating configurations, and lead to improved light extraction efficiency in LEDs.[32–35] The photonic crystal structure is periodic with translational symmetry. The periodic structure can exhibit a photonic band gap to inhibit the propagation of guided modes and uses a photonic crystal structure to couple guided modes with radiative modes.[36–39] Photonic crystal lasers based on the band-edge effect have several advantages, such as high-power emissions, single mode operation, and coherent oscillation.[40–43] E-beam lithography and laser interference lithography have been used to produce the photonic crystal structure.[44,45] Furthermore, because the emitting units are separated and the emission surfaces face each other, the light can be mixed effectively. Thus, nanorods are considered to have a great potential for improving the luminous efficiency in the green-to-red emission region, and numerous efforts have been adopted.[46, 47] However, nanoimprint lithography (NIL) offers high-level resolution, low-cost, and high throughput compared with other forms of lithography including laser interference and e-beam lithography.[48–50] In this study, we demonstrated the multiple color emission from a GaN-based 2D photonic quasicrystal (PQC) structure as illustrated in Fig. 1.The PQC structure was fabricated using NIL.[41,43] The total area of the PQC pattern is approximately 4 cm x 4 cm(2-in. sapphire substrate) and possessed 12-fold symmetry,[51,52] with a lattice constant of approximately 750 nm, a diameter of 300 nm and the depth of the nanopillars is approximately 1 μm. The PQC structure formed a complete band gap with the regrowth of 430-nm-tall GaN pyramids and 10-pair semipolar {10-11} In x Ga 1-x N/GaN (3 nm/12 nm) multiple quantum well (MQW) nanostructures, as illustrated in Fig. 1. Under room temperature pumping operation, the device demonstrates laser action with a low threshold power density and the multiple color emission simultaneously. We had reported the single color laser action from the GaN PQC structure.[41,43] This PQC platform exhibits the advantages in low fabrication costs, and better integration of GaN-based material with multi-color systems. In the future, the multiple-color GaN-based lasers can be expected with the optimization of regrowth procedure and the high quality photonic crystal cavity. Figure 2 illustrates the schematic procedures of the device fabrication. The fabrication procedures included epitaxial growth of a GaN wafer, NIL of PQC patterns, and dry etching. The GaN-based material was grown in a low-pressure metalorganic chemical vapor deposition reactor on a C-plane (0001) sapphire substrate. To prepare a clean surface of the sapphire substrate, the substrate was immersed into a burning solution of sulfuric acid: phosphoric acid = 3:1, then heat the beaker to a constant temperature for 1 hour. The substrate was cleaned with DI water under ultrasonic oscillation. A GaN (1-μm thick) was first grown on a 2-inch sapphire substrate at 1160°C. A 0.4-μm SiO 2 mask and 0.2-μm polymer mask were then deposited. After the polymer film was dry, a patterned mold of a 2-inch PQC structure was placed onto it by applying high pressure (Fig. 2. step 1). The substrate was heated to higher than the polymer’s glass transition temperature (T g ). The substrate and the mold were then cooled to room temperature to release the mold. The PQC patterns were defined on the polymer layer (Fig. 2, step 2). The patterns were then transferred into a SiO 2 layer with reactive ion etching (RIE) by using a CHF 3 /O 2 mixture (Fig. 2, step 3). The SiO 2 layer was used as a hard mask. The structure was then etched using inductively coupled plasma RIE with a Cl 2 /Ar mixture. The mask of SiO 2 layer was removed at the end of the etching process (Fig. 2, step 4). Before the regrowth process, the sample was passivated with porous SiO 2 at the sidewall. The pyramid-shaped GaN structures were regrown on top of the GaN nanopillars at 730°C. The 0.43-μm-high pyramids contained 10-pair In x Ga 1-x N/GaN (3 nm/12 nm) quantum wells, which supported different wavelengths of blue and green color emission, with the ratio of in composition: In x Ga 1-x N/GaN-dependent InN fraction variations. In 0.1 Ga 0.9 N/GaN MQWs and In 0.3 Ga 0.7 N/GaN MQWs corresponded to 460-and 520-nm emission wavelengths, respectively (Fig. 2, step 5). The etch depth of the nanorods was approximately 1 μm, as illustrated in Fig. 3(a). The PQC structure with porous SiO 2 at the sidewall and a semipolar {10-11} In x Ga 1-x N/GaN MQW are exhibited in the scattered electron microscopy (SEM) images in Fig. 3(b) (side view) and 3(c) (top-view). Figure 3(d) displays the magnification of semipolar {10-11} In x Ga 1-x N/GaN MQW with the facets of trapezoid microstructures. The semipolar {10-11} planes can reduce the influence of the quantum-confined Stark effect on the quantum efficiency of LEDs due to the surface stability and suppression of polarization effects.[53–56] To study the optical properties of the GaN-based PQC with nanopyramid structure, two GaN PQC samples were prepared: A, In 0.1 Ga 0.9 N/GaN MQWs, and B, In 0.3 Ga 0.7 N/GaN MQWs with regrowth fabrication. During the regrowth step, the temperature is the key to control the ratio of indium composition. The control temperature of blue In 0.1 Ga 0.9 N is 760~780°C and the control temperature of green In 0.3 Ga 0.7 N is 730~740°C. To demonstrate the optical mode from the photonic quasicrystal structure, samples A and B were optically pumped by a continuous-wave (CW) He-Cd laser at 325 nm with an incident power of approximately 50 mW. The light emission from the device was collected by a 15× objective lens through a multimode fiber, and coupled into a spectrometer with charge-coupled device detectors. Figure 4(a) illustrates the measured PL spectra under He-Cd 325 nm CW laser pumping. The spectrum of the black curve is the light emission with a wavelength of 366nm from the GaN-based PQC structure displayed in Fig. 3(a). Both samples A (blue curve) and B (green curve) had a strong emission peak which corresponded to wavelengths of approximately 460 and 520 nm respectively, resulting from the In x Ga 1-x N/GaN MQWs structure. The spectrum linewidths of the samples A and B were 40 and 60 nm, respectively. Figure 4(a) also displays photographs of the PQC structure of samples A and B during measurement. The CIE coordinates of PL from samples A and B were (0.19, 0.38) and (0.15, 0.07), respectively, as illustrated in Fig. 4(b). Thus, this hybrid platform has several possibilities for multicolor LEDs. It should be note that the peak of the sample B is broader than the one of sample A in Fig. 4(a). The slight broad spectrum from the sample B was attributed to the existence of defects and dislocations generated by the higher indium composition [57-59]. In order to confirm the optical resonant modes were the PQC band-edge modes, the finite-element method (FEM)[60, 61] was used to perform a simulation for the 12-fold symmetry photonic quasicrystal lattices. The calculated transmission spectra of the PQC with incident angles along with 0, 5°, 10°, 15°, 20°, and 25° as indicated in Fig. 5(a) was presented in Fig. 5(b). Due to the symmetry of this PQC lattices, the spectra would repeat for every 30° incident angle. The high transmission value in the spectra (blue color) indicate that the incident signal coupled into the PQC lattice resonant modes which are the band diagram areas. The low transmission (yellow color) regions indicate several photonic band gaps (PBGs) of the PQC structure. The ratio of high-to-low transmission is more than four order which show the PQC lattices take the strong effect to select the propagation modes in the device. The observed lasing actions occur around the band-edges of the PQC bandstructure, which are the boundaries between the high-transmission and low-transmission regimes in the Fig. 5(b). The flat dispersion curve near the band-edge implies a low group velocity of light and strong localization, and lead to the lasing actions of the devices. These PBGs matched the emission wavelength of In x Ga 1-x N/GaN with the corresponded normalized frequency are a/λ ≈ 0.88, 1.0, and 1.25 which were labeled as mode M 1 , M 2 , and M 3 . With the coupling between the PQC band-edge resonances and the emission from the InGaN/GaN layers, the emission efficiency and the light extraction at the specific wavelength would be further improved. The lasing action from GaN coupled to the high frequency M 3 could be achieved under sufficient excitation as our previous demonstration[43,45]. For the regrown In 0.1 Ga 0.9 N and In 0.3 Ga 0.7 N which coupled to M 2 and M 1 , the emission blue and green light would be boosted. Therefore, leveraging the coupling between the optical modes of PQC structure and In x Ga 1-x N/GaN, efficient multicolor LEDs, LDs could be realized in such hybrid platform. The length of the nanorods in photonic crystal lattices is also important to generate the high quality color enhancement. In this study, in order to achieve high quality color enhancement, the photonic crystal nanorod length was etched to 1000 nm which is more than four times of the effective wavelength. To realize the multicolor emission from a single PQC device in the future, the multiple regrowth procedures should be added in the epitaxial process. In summary, a 12-fold symmetric GaN PQC nanopillars was fabricated using the NIL technology. High-efficiency blue and green color emissions from In x Ga 1-x N/GaN MQWs were achieved with the regrowth procedure of the top In x Ga 1-x N/GaN MQWs grown on these facets, with an In composition ratio: In x Ga 1-x N/GaN-dependent InN fraction variations. The emission peaks were observed around 366-, 460-, and 520-nm wavelength resulting from In 0.1 Ga 0.9 N/GaN MQWs and In 0.3 Ga 0.7 N/GaN MQWs, respectively. These emission modes correspond to the band-edge resonant modes of the GaN PQC structure with FEM simulation. The methods of fabrication demonstrated a great potential to be a low-cost technique for fabricating semipolar {10-11} In x Ga 1-x N/GaN LED to use in manufacturing multicolor light sources. We believe that GaN-based photonic quasicrystal lasers could be integrated into multicolor light source systems in the future. Declarations Competing interests The authors declare that they have no competing interests. Authors' contributions CCC participated in the design of the study and measured the optical properties and drafted the manuscript. HTL calculated transmission spectrum of the 12-fold symmetry photonic quasicrystal lattices by FEM and helped to draft the manuscript. SPC carried out the study of ultraviolet GaN-based photonic quasicrystal nanopyramid structure and drafted the manuscript. HWH, KHC and YCC helped to fabricate the process of nanoimprint lithography, analyzed the optical properties, and helped to draft the manuscript. MHS and HCK conceived of the study, participated in its design and coordination, and helped draft the manuscript. All authors read and approved the final manuscript. Acknowledgements The authors are grateful to National Yang Ming Chiao Tung University’s Center for Nano Science and Technology, the financial support from the Bureau of Energy, Ministry of Economic Affairs and the Ministry of Science and Technology (MOST), Taiwan under Grant No. 108-2112-M-001-044-MY2 and 105-2112-M-001-011-MY3. Author details 1 Energy and Environment Research Laboratories, Industrial Technology Research Institute, Hsinchu 31040, Taiwan 2 Research Center for Applied Sciences (RCAS), Academia Sinica, Taipei 11529, Taiwan 3 Department of Photonics and Institute of Electro-Optical Engineering, National Chiao Tung University, Hsinchu 30010, Taiwan References Nakamura S, Mukai T, Senoh M:Candela‐class high‐brightness InGaN/AlGaN double‐heterostructure blue‐light‐emitting diodes. Appl Phys Lett 1994, 64: 1687-1689. Nakamura S, Senoh M, Iwasa N, Nagahama S:High-Brightness InGaN Blue, Green and Yellow Light-Emitting Diodes with Quantum Well Structures. Jpn J Appl Phys 1995, 34: L797-L799. Nakamura S, Senoh M, Nagahama SI, Iwasa N, Yamada T, Matsushita T, Sugimoto Y, Kiyoku H: Room-temperature continuous-wave operation of InGaN multi-quantum-well-structure laser diodes with a long lifetime. Appl Phys Lett 1997, 70: 868-870. 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Cite Share Download PDF Status: Under Review Version 1 posted Reviews received at journal 06 Jun, 2021 Reviewers invited by journal 03 Jun, 2021 Editor assigned by journal 03 Jun, 2021 First submitted to journal 26 May, 2021 Editorial decision: Minor revision 06 Aug, 2020 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-320128","acceptedTermsAndConditions":true,"allowDirectSubmit":false,"archivedVersions":[],"articleType":"Research Article","associatedPublications":[],"authors":[{"id":31297401,"identity":"406985b6-a67c-4a84-9640-1956dcdb77d4","order_by":0,"name":"Cheng-Chang Chen","email":"data:image/png;base64,iVBORw0KGgoAAAANSUhEUgAAAZAAAAAyAQMAAABI0h/eAAAABlBMVEX///8AAABVwtN+AAAACXBIWXMAAA7EAAAOxAGVKw4bAAAAwklEQVRIiWNgGAWjYDACCTBpw8PAwNhAkpY0Hh6YFh4itRxGqCSohX9287EHP2rOy9hLH25g+LinlsFeIoGAJXeOpRv2HLvNw8OX2MA449lxBh5CWgwkcsykGRuAWngYG5h5Dhxj4JEmqCX/G1DLOZK05LABtRyAaakhrEXiRpqZZM+xZB6eM4wNB2ccAOq9/wC/Fv4Zyc8kftTY2bP3sD988OFAnRx7zwH8WlAAUO1hwjGJDupI1jEKRsEoGAXDHwAA3Uk57sy3/ScAAAAASUVORK5CYII=","orcid":"","institution":"Industrial Technology Research Instutude","correspondingAuthor":true,"submittingAuthor":false,"prefix":"","firstName":"Cheng-Chang","middleName":"","lastName":"Chen","suffix":""},{"id":31297402,"identity":"5b56d92c-e9b2-4af6-a27d-119abf785572","order_by":1,"name":"Hsiang-Ting Lin","email":"","orcid":"","institution":"Research Center for Applied Sciences, Academia Sinica, Taipei","correspondingAuthor":false,"submittingAuthor":false,"prefix":"","firstName":"Hsiang-Ting","middleName":"","lastName":"Lin","suffix":""},{"id":31297403,"identity":"91da21a2-efc3-4464-a601-edaa72713822","order_by":2,"name":"Shih-Pang Chang","email":"","orcid":"","institution":"Department of Photonics and Institute of Electro-Optical Engineering, National Chiao Tung University","correspondingAuthor":false,"submittingAuthor":false,"prefix":"","firstName":"Shih-Pang","middleName":"","lastName":"Chang","suffix":""},{"id":31297404,"identity":"432ec259-fa05-43e6-b4a3-706eede44f84","order_by":3,"name":"Hao-Chung Kuo","email":"","orcid":"","institution":"Department of Photonics and Institute of Electro-Optical Engineering, National Chiao Tung University","correspondingAuthor":false,"submittingAuthor":false,"prefix":"","firstName":"Hao-Chung","middleName":"","lastName":"Kuo","suffix":""},{"id":31297405,"identity":"27de5693-6f27-48bd-bb54-2c39ad90ccfd","order_by":4,"name":"Hsiao-Wen Hung","email":"","orcid":"","institution":"Energy and Environment Research Laboratories, Industrial Technology Research Institute","correspondingAuthor":false,"submittingAuthor":false,"prefix":"","firstName":"Hsiao-Wen","middleName":"","lastName":"Hung","suffix":""},{"id":31297406,"identity":"52466b11-f0dd-4e6f-833f-323dfd93add5","order_by":5,"name":"Kuo-Hsiang Chien","email":"","orcid":"","institution":"Energy and Environment Research Laboratories, Industrial Technology Research Institute","correspondingAuthor":false,"submittingAuthor":false,"prefix":"","firstName":"Kuo-Hsiang","middleName":"","lastName":"Chien","suffix":""},{"id":31297407,"identity":"321cabbd-715e-4f89-8635-89311ea4594e","order_by":6,"name":"Yu-Choung Chang","email":"","orcid":"","institution":"Energy and environment Research Laboratories, Industrial Technology Research Institute","correspondingAuthor":false,"submittingAuthor":false,"prefix":"","firstName":"Yu-Choung","middleName":"","lastName":"Chang","suffix":""},{"id":31297408,"identity":"cf744faf-eb56-4bfc-865f-16e88fc544d6","order_by":7,"name":"Min-Hsiung Shih","email":"","orcid":"","institution":"Academia Sinica","correspondingAuthor":false,"submittingAuthor":false,"prefix":"","firstName":"Min-Hsiung","middleName":"","lastName":"Shih","suffix":""}],"badges":[],"createdAt":"2021-03-12 09:38:56","currentVersionCode":1,"declarations":"","doi":"10.21203/rs.3.rs-320128/v1","doiUrl":"https://doi.org/10.21203/rs.3.rs-320128/v1","draftVersion":[],"editorialEvents":[],"editorialNote":"","failedWorkflow":false,"files":[{"id":10075846,"identity":"b2c71b2d-9e01-497b-be44-2c33c614ab7a","added_by":"auto","created_at":"2021-06-07 16:33:30","extension":"jpg","order_by":1,"title":"Figure 1","display":"","copyAsset":false,"role":"figure","size":124574,"visible":true,"origin":"","legend":"Schematic structure of GaN-based PQC structure with the regrowth of semipolar {10-11} GaN pyramids and 10-pair InxGa1-xN/GaN (3 nm/12 nm) MQW.","description":"","filename":"1.jpg","url":"https://assets-eu.researchsquare.com/files/rs-320128/v1/73402bc4660c2c46fa9a4209.jpg"},{"id":10075587,"identity":"753af842-9f2b-460b-9348-0198dc0b9a12","added_by":"auto","created_at":"2021-06-07 16:30:30","extension":"jpg","order_by":2,"title":"Figure 2","display":"","copyAsset":false,"role":"figure","size":66414,"visible":true,"origin":"","legend":"Schematic of fabrication process. The fabrication procedures of the GaN PQC structure. Including epitaxial growth of a GaN wafer (step 1), NIL of PQC patterns (step 2), dry etching (steps 3 and 4), and pyramid-on-nanorods MQW structure after regrowth (step 5).","description":"","filename":"2.jpg","url":"https://assets-eu.researchsquare.com/files/rs-320128/v1/565b102354df94b57ae1a76b.jpg"},{"id":10075983,"identity":"61be32e0-c496-40a8-b205-e1e76af3d8e6","added_by":"auto","created_at":"2021-06-07 16:36:30","extension":"jpg","order_by":3,"title":"Figure 3","display":"","copyAsset":false,"role":"figure","size":83096,"visible":true,"origin":"","legend":"(a) Tile angle-view SEM image of the PQC structure. (b) Sidewall of the SEM image of the PQC structure with porous SiO2. (c) Top-view SEM image of the PQC structure after the regrowth procedure. (d) Magnifying SEM image of semipolar {10-11} InxGa1-xN/GaN MQW with the facets of trapezoid microstructures.","description":"","filename":"3.jpg","url":"https://assets-eu.researchsquare.com/files/rs-320128/v1/cfbec95dc1180aa9680f89e5.jpg"},{"id":10075845,"identity":"2af46ddf-a2f0-488d-9437-2c3fcba5b8ba","added_by":"auto","created_at":"2021-06-07 16:33:30","extension":"jpg","order_by":4,"title":"Figure 4","display":"","copyAsset":false,"role":"figure","size":70409,"visible":true,"origin":"","legend":"(a) PL spectra from the nanorods of GaN-based material (black), samples A (blue) and B (green). (b) Photographs of the PQC structure of samples A and B during measurement corresponding to the CIE coordinates of (0.19, 0.38) and (0.15, 0.07), respectively.","description":"","filename":"4.jpg","url":"https://assets-eu.researchsquare.com/files/rs-320128/v1/e0968992236e298becb74bef.jpg"},{"id":10075589,"identity":"3990af83-41fc-4ce8-922e-f2bd2adc2e20","added_by":"auto","created_at":"2021-06-07 16:30:30","extension":"jpg","order_by":5,"title":"Figure 5","display":"","copyAsset":false,"role":"figure","size":49470,"visible":true,"origin":"","legend":"(a) Duplicate spectra for every 30° incident angle owing to the symmetry of the PQC structure. (b) Transmission spectrum of the 12-fold symmetry photonic quasicrystal lattices, calculated by FEM corresponding to different band-edge resonant modes.","description":"","filename":"5.jpg","url":"https://assets-eu.researchsquare.com/files/rs-320128/v1/9dec791b6c22055949a2bb90.jpg"},{"id":15672872,"identity":"b7100263-e8bd-45e8-b23f-eaab0e93eb38","added_by":"auto","created_at":"2021-11-18 14:14:47","extension":"pdf","order_by":0,"title":"","display":"","copyAsset":false,"role":"manuscript-pdf","size":451218,"visible":true,"origin":"","legend":"","description":"","filename":"manuscript.pdf","url":"https://assets-eu.researchsquare.com/files/rs-320128/v1/740584bb-8582-426e-b870-7816b892acd1.pdf"}],"financialInterests":"","formattedTitle":"\u003cp\u003eMulticolor Emission from Ultraviolet GaN-based Photonic Quasicrystal Nanopyramid Structure with Semipolar In\u003csub\u003ex\u003c/sub\u003eGa\u003csub\u003e1-x\u003c/sub\u003eN/GaN Multiple Quantum Wells\u003c/p\u003e","fulltext":[{"header":"Main Text","content":"\u003cp\u003eThe potential applications of GaN-based materials have recently attracted attention because of their large direct band gap and their potential for use in optoelectronic devices, including light emitting diodes (LEDs)[1-3] and laser diodes (LDs).[4-5] GaN-based LEDs have been applied in traffic signals, display backlights,[6-8] solid-state lighting,[9,10] biosensors,[11] and optogenetics.[12] A potential applications for GaN-based LEDs would be in the development of phosphor-free white LEDs, including multichip white LEDs, monolithic LEDs, and color-conversion white LEDs.[13,14] Blue LD can serve as the light source for high-density data storage in a Blu-ray Disc (BD), which is a popular data storage tool. Promoting and increasing the efficiency of the light source is imperative because of its multitude of potential applications. GaN-based nanorods possess low dislocation, low internal field, and high light extraction efficiency, which are the factors intrinsic in improving photoluminescence (PL) intensity.[15,16] Various approaches have been employed to increase the light extraction efficiency for III-nitride LEDs, such as rough surfaces,[17-20] sapphire microlenses,[21] oblique mesa sidewalls,[22] nanopyramids,[23] graded refractive index materials,[24] self-assembled lithography patterning,[25] colloidal-based microlens arrays,[26,27] and photonic crystals.[28\u0026ndash;31] Photonic crystals have been reported in quasicrystal or defective two-dimensional (2D) grating configurations, and lead to improved light extraction efficiency in LEDs.[32\u0026ndash;35] The photonic crystal structure is periodic with translational symmetry. The periodic structure can exhibit a photonic band gap to inhibit the propagation of guided modes and uses a photonic crystal structure to couple guided modes with radiative modes.[36\u0026ndash;39] Photonic crystal lasers based on the band-edge effect have several advantages, such as high-power emissions, single mode operation, and coherent oscillation.[40\u0026ndash;43] E-beam lithography and laser interference lithography have been used to produce the photonic crystal structure.[44,45] Furthermore, because the emitting units are separated and the emission surfaces face each other, the light can be mixed effectively. Thus, nanorods are considered to have a great potential for improving the luminous efficiency in the green-to-red emission region, and numerous efforts have been adopted.[46, 47]\u003c/p\u003e\n\u003cp\u003eHowever, nanoimprint lithography (NIL) offers high-level resolution, low-cost, and high throughput compared with other forms of lithography including laser interference and e-beam lithography.[48\u0026ndash;50] In this study, we demonstrated the multiple color emission from a GaN-based 2D photonic quasicrystal (PQC) structure as illustrated in Fig. 1.The PQC structure was fabricated using NIL.[41,43] The total area of the PQC pattern is approximately 4 cm x 4 cm(2-in. sapphire substrate) and possessed 12-fold symmetry,[51,52] with a lattice constant of approximately 750 nm, a diameter of 300 nm and the depth of the nanopillars is approximately 1 \u0026mu;m. The PQC structure formed a complete band gap with the regrowth of 430-nm-tall GaN pyramids and 10-pair semipolar {10-11} In\u003csub\u003ex\u003c/sub\u003eGa\u003csub\u003e1-x\u003c/sub\u003eN/GaN (3 nm/12 nm) multiple quantum well (MQW) nanostructures, as illustrated in Fig. 1.\u003c/p\u003e\n\u003cp\u003eUnder room temperature pumping operation, the device demonstrates laser action with a low threshold power density and the multiple color emission simultaneously. We had reported the single color laser action from the GaN PQC structure.[41,43] This PQC platform exhibits the advantages in low fabrication costs, and better integration of GaN-based material with multi-color systems. In the future, the multiple-color GaN-based lasers can be expected with the optimization of regrowth procedure and the high quality photonic crystal cavity.\u003c/p\u003e\n\u003cp\u003eFigure 2 illustrates the schematic procedures of the device fabrication. The fabrication procedures included epitaxial growth of a GaN wafer, NIL of PQC patterns, and dry etching. The GaN-based material was grown in a low-pressure metalorganic chemical vapor deposition reactor on a C-plane (0001) sapphire substrate. To prepare a clean surface of the sapphire substrate, the substrate was immersed into a burning solution of sulfuric acid: phosphoric acid = 3:1, then heat the beaker to a constant temperature for 1 hour. The substrate was cleaned with DI water under ultrasonic oscillation. A GaN (1-\u0026mu;m thick) was first grown on a 2-inch sapphire substrate at 1160\u0026deg;C. A 0.4-\u0026mu;m SiO\u003csub\u003e2\u003c/sub\u003e mask and 0.2-\u0026mu;m polymer mask were then deposited. After the polymer film was dry, a patterned mold of a 2-inch PQC structure was placed onto it by applying high pressure (Fig. 2. step 1). The substrate was heated to higher than the polymer\u0026rsquo;s glass transition temperature (T\u003csub\u003eg\u003c/sub\u003e). The substrate and the mold were then cooled to room temperature to release the mold. The PQC patterns were defined on the polymer layer (Fig. 2, step 2). The patterns were then transferred into a SiO\u003csub\u003e2\u003c/sub\u003e layer with reactive ion etching (RIE) by using a CHF\u003csub\u003e3\u003c/sub\u003e/O\u003csub\u003e2 \u003c/sub\u003emixture (Fig. 2, step 3). The SiO\u003csub\u003e2 \u003c/sub\u003elayer was used as a hard mask. The structure was then etched using inductively coupled plasma RIE with a Cl\u003csub\u003e2\u003c/sub\u003e/Ar mixture. The mask of SiO\u003csub\u003e2\u003c/sub\u003e layer was removed at the end of the etching process (Fig. 2, step 4).\u003c/p\u003e\n\u003cp\u003eBefore the regrowth process, the sample was passivated with porous SiO\u003csub\u003e2\u003c/sub\u003e at the sidewall. The pyramid-shaped GaN structures were regrown on top of the GaN nanopillars at 730\u0026deg;C. The 0.43-\u0026mu;m-high pyramids contained 10-pair In\u003csub\u003ex\u003c/sub\u003eGa\u003csub\u003e1-x\u003c/sub\u003e N/GaN (3 nm/12 nm) quantum wells, which supported different wavelengths of blue and green color emission, with the ratio of in composition: In\u003csub\u003ex\u003c/sub\u003eGa\u003csub\u003e1-x\u003c/sub\u003eN/GaN-dependent InN fraction variations. In\u003csub\u003e0.1\u003c/sub\u003eGa\u003csub\u003e0.9\u003c/sub\u003eN/GaN MQWs and In\u003csub\u003e0.3\u003c/sub\u003eGa\u003csub\u003e0.7\u003c/sub\u003eN/GaN MQWs\u003cem\u003e corresponded to \u003c/em\u003e460-and 520-nm emission wavelengths, respectively (Fig. 2, step 5). The etch depth of the nanorods was approximately 1 \u0026mu;m, as illustrated in Fig. 3(a). The PQC structure with porous SiO\u003csub\u003e2\u003c/sub\u003e at the sidewall and a semipolar {10-11} In\u003csub\u003ex\u003c/sub\u003eGa\u003csub\u003e1-x\u003c/sub\u003e N/GaN MQW are exhibited in the scattered electron microscopy (SEM) images in Fig. 3(b) (side view) and 3(c) (top-view). Figure 3(d) displays the magnification of semipolar {10-11} In\u003csub\u003ex\u003c/sub\u003eGa\u003csub\u003e1-x\u003c/sub\u003e N/GaN MQW with the facets of trapezoid microstructures. The semipolar {10-11} planes can reduce the influence of the quantum-confined Stark effect on the quantum efficiency of LEDs due to the surface stability and suppression of polarization effects.[53\u0026ndash;56]\u003c/p\u003e\n\u003cp\u003eTo study the optical properties of the GaN-based PQC with nanopyramid structure, two GaN PQC samples were prepared: A, In\u003csub\u003e0.1\u003c/sub\u003eGa\u003csub\u003e0.9\u003c/sub\u003eN/GaN MQWs, and B, In\u003csub\u003e0.3\u003c/sub\u003eGa\u003csub\u003e0.7\u003c/sub\u003eN/GaN MQWs with regrowth fabrication. During the regrowth step, the temperature is the key to control the ratio of indium composition. The control temperature of blue In\u003csub\u003e0.1\u003c/sub\u003eGa\u003csub\u003e0.9\u003c/sub\u003eN is 760~780\u0026deg;C and the control temperature of green In\u003csub\u003e0.3\u003c/sub\u003eGa\u003csub\u003e0.7\u003c/sub\u003eN is 730~740\u0026deg;C. To demonstrate the optical mode from the photonic quasicrystal structure, samples A and B were optically pumped by a continuous-wave (CW) He-Cd laser at 325 nm with an incident power of approximately 50 mW. The light emission from the device was collected by a 15\u0026times; objective lens through a multimode fiber, and coupled into a spectrometer with charge-coupled device detectors. Figure 4(a) illustrates the measured PL spectra under He-Cd 325 nm CW laser pumping. The spectrum of the black curve is the light emission with a wavelength of 366nm from the GaN-based PQC structure displayed in Fig. 3(a). Both samples A (blue curve) and B (green curve) had a strong emission peak which corresponded to wavelengths of approximately 460 and 520 nm respectively, resulting from the In\u003csub\u003ex\u003c/sub\u003eGa\u003csub\u003e1-x\u003c/sub\u003e N/GaN MQWs structure. The spectrum linewidths of the samples A and B were 40 and 60 nm, respectively. Figure 4(a) also displays photographs of the PQC structure of samples A and B during measurement. The CIE coordinates of PL from samples A and B were (0.19, 0.38) and (0.15, 0.07), respectively, as illustrated in Fig. 4(b). Thus, this hybrid platform has several possibilities for multicolor LEDs. It should be note that the peak of the sample B is broader than the one of sample A in Fig. 4(a). The slight broad spectrum from the sample B was attributed to the existence of defects and dislocations generated by the higher indium composition [57-59].\u003c/p\u003e\n\u003cp\u003eIn order to confirm the optical resonant modes were the PQC band-edge modes, the finite-element method (FEM)[60, 61] was used to perform a simulation for the 12-fold symmetry photonic quasicrystal lattices. The calculated transmission spectra of the PQC with incident angles along with 0, 5\u0026deg;, 10\u0026deg;, 15\u0026deg;, 20\u0026deg;, and 25\u0026deg; as indicated in Fig. 5(a) was presented in Fig. 5(b). Due to the symmetry of this PQC lattices, the spectra would repeat for every 30\u0026deg; incident angle. The high transmission value in the spectra (blue color) indicate that the incident signal coupled into the PQC lattice resonant modes which are the band diagram areas. The low transmission (yellow color) regions indicate several photonic band gaps (PBGs) of the PQC structure. The ratio of high-to-low transmission is more than four order which show the PQC lattices take the strong effect to select the propagation modes in the device. The observed lasing actions occur around the band-edges of the PQC bandstructure, which are the boundaries between the high-transmission and low-transmission regimes in the Fig. 5(b). The flat dispersion curve near the band-edge implies a low group velocity of light and strong localization, and lead to the lasing actions of the devices. These PBGs matched the emission wavelength of In\u003csub\u003ex\u003c/sub\u003eGa\u003csub\u003e1-x\u003c/sub\u003eN/GaN with the corresponded normalized frequency are a/\u0026lambda; \u0026asymp; 0.88, 1.0, and 1.25 which were labeled as mode M\u003csub\u003e1\u003c/sub\u003e, M\u003csub\u003e2\u003c/sub\u003e, and M\u003csub\u003e3\u003c/sub\u003e. With the coupling between the PQC band-edge resonances and the emission from the InGaN/GaN layers, the emission efficiency and the light extraction at the specific wavelength would be further improved. The lasing action from GaN coupled to the high frequency M\u003csub\u003e3\u003c/sub\u003e could be achieved under sufficient excitation as our previous demonstration[43,45]. For the regrown In\u003csub\u003e0.1\u003c/sub\u003eGa\u003csub\u003e0.9\u003c/sub\u003eN and In\u003csub\u003e0.3\u003c/sub\u003eGa\u003csub\u003e0.7\u003c/sub\u003eN which coupled to M\u003csub\u003e2\u003c/sub\u003e and M\u003csub\u003e1\u003c/sub\u003e, the emission blue and green light would be boosted. Therefore, leveraging the coupling between the optical modes of PQC structure and In\u003csub\u003ex\u003c/sub\u003eGa\u003csub\u003e1-x\u003c/sub\u003eN/GaN, efficient multicolor LEDs, LDs could be realized in such hybrid platform. The length of the nanorods in photonic crystal lattices is also important to generate the high quality color enhancement. In this study, in order to achieve high quality color enhancement, the photonic crystal nanorod length was etched to 1000 nm which is more than four times of the effective wavelength. To realize the multicolor emission from a single PQC device in the future, the multiple regrowth procedures should be added in the epitaxial process.\u003c/p\u003e\n\u003cp\u003eIn summary, a 12-fold symmetric GaN PQC nanopillars was fabricated using the NIL technology. High-efficiency blue and green color emissions from In\u003csub\u003ex\u003c/sub\u003eGa\u003csub\u003e1-x\u003c/sub\u003eN/GaN MQWs were achieved with the regrowth procedure of the top In\u003csub\u003ex\u003c/sub\u003eGa\u003csub\u003e1-x\u003c/sub\u003eN/GaN MQWs grown on these facets, with an In composition ratio: In\u003csub\u003ex\u003c/sub\u003eGa\u003csub\u003e1-x\u003c/sub\u003eN/GaN-dependent InN fraction variations. The emission peaks were observed around 366-, 460-, and 520-nm wavelength resulting from In\u003csub\u003e0.1\u003c/sub\u003eGa\u003csub\u003e0.9\u003c/sub\u003eN/GaN MQWs and In\u003csub\u003e0.3\u003c/sub\u003eGa\u003csub\u003e0.7\u003c/sub\u003eN/GaN MQWs, respectively. These emission modes correspond to the band-edge resonant modes of the GaN PQC structure with FEM simulation. The methods of fabrication demonstrated a great potential to be a low-cost technique for fabricating semipolar {10-11} In\u003csub\u003ex\u003c/sub\u003eGa\u003csub\u003e1-x\u003c/sub\u003eN/GaN LED to use in manufacturing multicolor light sources. We believe that GaN-based photonic quasicrystal lasers could be integrated into multicolor light source systems in the future.\u003c/p\u003e"},{"header":"Declarations","content":"\u003cp\u003e\u003cstrong\u003eCompeting interests\u003c/strong\u003e\u003c/p\u003e\n\u003cp\u003eThe authors declare that they have no competing interests.\u003c/p\u003e\n\u003cp\u003e\u003cstrong\u003eAuthors' contributions\u003c/strong\u003e\u003c/p\u003e\n\u003cp\u003eCCC participated in the design of the study and measured the optical properties and drafted the manuscript. HTL calculated transmission spectrum of the 12-fold symmetry photonic quasicrystal lattices by FEM and helped to draft the manuscript. SPC carried out the study of ultraviolet GaN-based photonic quasicrystal nanopyramid structure and drafted the manuscript. HWH, KHC and YCC helped to fabricate the process of nanoimprint lithography, analyzed the optical properties, and helped to draft the manuscript. MHS and HCK conceived of the study, participated in its design and coordination, and helped draft the manuscript. All authors read and approved the final manuscript.\u003c/p\u003e\n\u003cp\u003e\u003cstrong\u003eAcknowledgements\u003c/strong\u003e\u003c/p\u003e\n\u003cp\u003eThe authors are grateful to National Yang Ming Chiao Tung University\u0026rsquo;s Center for Nano Science and Technology, the financial support from the Bureau of Energy, Ministry of Economic Affairs and the Ministry of Science and Technology (MOST), Taiwan under Grant No. 108-2112-M-001-044-MY2 and 105-2112-M-001-011-MY3.\u003c/p\u003e\n\u003cp\u003e\u003cstrong\u003eAuthor details\u003c/strong\u003e\u003c/p\u003e\n\u003cp\u003e\u003csup\u003e1\u003c/sup\u003eEnergy and Environment Research Laboratories, Industrial Technology Research Institute, Hsinchu 31040, Taiwan\u003c/p\u003e\n\u003cp\u003e\u003csup\u003e2\u003c/sup\u003eResearch Center for Applied Sciences (RCAS), Academia Sinica, Taipei 11529, Taiwan\u003c/p\u003e\n\u003cp\u003e\u003csup\u003e3\u003c/sup\u003eDepartment of Photonics and Institute of Electro-Optical Engineering, National Chiao Tung University, Hsinchu 30010, Taiwan\u003c/p\u003e"},{"header":"References","content":"\u003col\u003e\n\u003cli\u003e\u003ca href=\"https://aip.scitation.org/author/Nakamura%2C+Shuji\"\u003eNakamura\u003c/a\u003e S,\u0026nbsp;\u003ca href=\"https://aip.scitation.org/author/Mukai%2C+Takashi\"\u003eMukai\u003c/a\u003e T, \u003ca href=\"https://aip.scitation.org/author/Senoh%2C+Masayuki\"\u003eSenoh\u003c/a\u003e M:Candela‐class high‐brightness InGaN/AlGaN double‐heterostructure blue‐light‐emitting diodes. 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Garcia-Adeva: The finite element method applied to the study of two-dimensional photonic crystals and resonant cavities. Opt. Express 2013, 21: 4072-4092.\u003c/li\u003e\n\u003c/ol\u003e"}],"fulltextSource":"","fullText":"","funders":[],"hasAdminPriorityOnWorkflow":false,"hasManuscriptDocX":true,"hasOptedInToPreprint":true,"hasPassedJournalQc":"","hasAnyPriority":false,"hideJournal":false,"highlight":"","institution":"","isAcceptedByJournal":true,"isAuthorSuppliedPdf":false,"isDeskRejected":"","isHiddenFromSearch":false,"isInQc":false,"isInWorkflow":false,"isPdf":false,"isPdfUpToDate":true,"isWithdrawnOrRetracted":false,"journal":{"display":true,"email":"[email protected]","identity":"discover-nano","isNatureJournal":false,"hasQc":true,"allowDirectSubmit":false,"externalIdentity":"narl","sideBox":"Learn more about [Discover Nano](https://www.springer.com/journal/11671)","snPcode":"11671","submissionUrl":"https://submission.nature.com/new-submission/11671/3","title":"Discover Nano","twitterHandle":"@SpringerOpen","acdcEnabled":true,"dfaEnabled":true,"editorialSystem":"stoa","reportingPortfolio":"Discover Series","inReviewEnabled":true,"inReviewRevisionsEnabled":true},"keywords":"GaN, GaN-based LEDs, Photonic quasicrystal multicolor emission, Finite-element method","lastPublishedDoi":"10.21203/rs.3.rs-320128/v1","lastPublishedDoiUrl":"https://doi.org/10.21203/rs.3.rs-320128/v1","license":{"name":"CC BY 4.0","url":"https://creativecommons.org/licenses/by/4.0/"},"manuscriptAbstract":"\u003cp\u003eIn this study, we demonstrated large-area high quality multi-color emission from the 12-fold symmetric GaN photonic quasicrystal nanorod device which was fabricated using the nanoimprint lithography technology and multiple quantum wells regrowth procedure. High-efficiency blue and green color emission wavelengths of 460 and 520 nm from the regrown In\u003csub\u003ex\u003c/sub\u003eGa\u003csub\u003e1\u0026minus;x\u003c/sub\u003eN/GaN multiple quantum wells were observed under optical pumping conditions. To confirm the strongly coupling between the quantum well emissions and the photonic crystal band-edge resonant modes, the finite-element method (FEM) was applied to perform a simulation of the 12-fold symmetry photonic quasicrystal lattices.\u003c/p\u003e","manuscriptTitle":"Multicolor Emission from Ultraviolet GaN-based Photonic Quasicrystal Nanopyramid Structure with Semipolar InxGa1-xN/GaN Multiple Quantum Wells","msid":"","msnumber":"","nonDraftVersions":[{"code":1,"date":"2021-06-07 16:30:28","doi":"10.21203/rs.3.rs-320128/v1","editorialEvents":[{"type":"communityComments","content":0},{"type":"editorInvitedReview","content":"","date":"2021-06-06T09:48:00+00:00","index":0,"fulltext":""},{"type":"reviewersInvited","content":"","date":"2021-06-03T23:25:00+00:00","index":"","fulltext":""},{"type":"editorAssigned","content":"","date":"2021-06-03T21:38:00+00:00","index":"","fulltext":""},{"type":"submitted","content":"Nanoscale Research Letters","date":"2021-05-27T02:35:17+00:00","index":"","fulltext":""},{"type":"decision","content":"Minor revision","date":"2020-08-06T09:22:42+00:00","index":"","fulltext":""}],"status":"published","journal":{"display":true,"email":"[email protected]","identity":"discover-nano","isNatureJournal":false,"hasQc":true,"allowDirectSubmit":false,"externalIdentity":"narl","sideBox":"Learn more about [Discover Nano](https://www.springer.com/journal/11671)","snPcode":"11671","submissionUrl":"https://submission.nature.com/new-submission/11671/3","title":"Discover Nano","twitterHandle":"@SpringerOpen","acdcEnabled":true,"dfaEnabled":true,"editorialSystem":"stoa","reportingPortfolio":"Discover Series","inReviewEnabled":true,"inReviewRevisionsEnabled":true}}],"origin":"","ownerIdentity":"c7e197db-33af-4086-b45b-b9092e6e6007","owner":[],"postedDate":"June 7th, 2021","published":true,"recentEditorialEvents":[],"rejectedJournal":[],"revision":"","amendment":"","status":"under-review","subjectAreas":[{"id":4852611,"name":"Nanoscience"}],"tags":[],"updatedAt":"2021-07-22T00:38:21+00:00","versionOfRecord":[],"versionCreatedAt":"2021-06-07 16:30:28","video":"","vorDoi":"","vorDoiUrl":"","workflowStages":[]},"version":"v1","identity":"rs-320128","journalConfig":"researchsquare"},"__N_SSP":true},"page":"/article/[identity]/[[...version]]","query":{"redirect":"/article/rs-320128","identity":"rs-320128","version":["v1"]},"buildId":"WrCJVZZCHTDjtuVLN7oU0","isFallback":false,"isExperimentalCompile":false,"dynamicIds":[84888],"gssp":true,"scriptLoader":[]}