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Ultrathin GaN Crystal Realized Through Nitrogen Substitution of Layered GaS

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Abstract

GaN has been demonstrated as an important wide-bandgap semiconductor in many applications, especially in optoelectronic and high-power electronics. Two-dimensional (2D) GaN, with increased bandgap compared to the bulk counterpart, not only amplifies existing functionalities but also opens up fresh possibilities for compact electronics. Although several methods have recently been developed to synthesize 2D GaN, their practical application is hampered by either harsh growth conditions (e.g., high temperature and ultrahigh vacuum) or unsatisfactory performance due to grain boundaries. Here, we report the realization of few-nanometer-thick GaN crystals via in situ atomic substitution of layered GaS flakes at a relatively low temperature (590°C). GaN with tunable thickness from 50 nm down to 0.9 nm (~2 atomic layers) is achieved by applying the atomic substitution reaction to GaS with different numbers of layers. The obtained ultrathin GaN flakes retain the morphology inherited from the GaS flakes and show high crystallinity by transmission electron microscopy (TEM) characterization, while the thickness of GaN decreases to about 72% of the corresponding GaS flakes from the atomic force microscopy characterization. A time-dependent mechanism study reveals both horizontal and vertical conversion paths, with Ga2S3 as intermediate. Photoluminescence (PL) spectroscopy measurements show that the band edge PL of 2D ultrathin GaN is blue-shifted as compared with bulk GaN, suggesting that the bandgap increases with the decrease in thickness. This study provides a promising method for obtaining ultrathin, high-crystallinity GaN with tunable thicknesses, utilizing a minimal thermal budget. This breakthrough lays a solid foundation for future investigations into fundamental physics and potential device applications.

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Acknowledgments

This research is primarily supported by the U.S. Department of Energy (DOE), Office of Science, Basic Energy Sciences (BES), under Award DE-SC0021064. X.L. and J.C. also acknowledge the support of Semiconductor Research Cooperation (SRC) under Award S4994. Work by W.J.L. and X.L. was supported by the National Science Foundation (NSF) under Grant No. (1945364). X.L. acknowledges the membership of the Photonics Center at Boston University. H.Z.G. acknowledges the support of a BUnano Cross-Disciplinary Fellowship. P.T. acknowledges the National Natural Science Foundation of China (Grant No. 11874350) and CAS Key Research Program of Frontier Sciences (Grant No. ZDBS-LY-SLH004). Some of the TEM imaging was performed at the Center for Nanoscale Systems (CNS), a member of the National Nanotechnology Coordinated Infrastructure Network (NNCI), which is supported by the National Science Foundation under NSF award no. 1541959. CNS is part of Harvard University. Work at the Molecular Foundry was supported by the Office of Science, Office of Basic Energy Sciences, of the U.S. Department of Energy under Contract No. DE-AC02-05CH11231. This material is based upon work supported by the U.S. Department of Energy, Office of Science, Office of Workforce Development for Teachers and Scientists, Office of Science Graduate Student Research (SCGSR) program. The SCGSR program is administered by the Oak Ridge Institute for Science and Education for the DOE under contract number DE-SC0014664. QM acknowledges support from the NSF Career program (award number DMR-2143426) and the CIFAR Azrieli Global Scholars program. We acknowledge Dr. X. An and Dr. B. M. Reinhard for help with SEM and EDS measurements.

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Authors and Affiliations

  1. Department of Chemistry, Boston University, 590 Commonwealth Avenue, Boston, MA, 02215, USA

    Jun Cao, Hongze Gao, Weijun Luo, Zifan Wang & Xi Ling

  2. Division of Materials Science and Engineering, Boston University, 15 St. Mary’s Street, Boston, MA, 02215, USA

    Tianshu Li & Xi Ling

  3. State Key Laboratory of Superlattices and Microstructures, Institute of Semiconductors, Chinese Academy of Sciences, Beijing, 100083, People’s Republic of China

    Xin Cong, Miao-Ling Lin & Ping-Heng Tan

  4. Department of Physics, Boston University, 590 Commonwealth Avenue, Boston, MA, 02215, USA

    Nicholas Russo & Kevin E. Smith

  5. Department of Physics, Boston College, Chestnut Hill, MA, 02467, USA

    Siyuan Ding & Qiong Ma

  6. The Photonics Center, Boston University, 8 St. Mary’s Street, Boston, MA, 02215, USA

    Xi Ling

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  1. Jun Cao
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Correspondence to Xi Ling.

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Cao, J., Li, T., Gao, H. et al. Ultrathin GaN Crystal Realized Through Nitrogen Substitution of Layered GaS. J. Electron. Mater. 52, 7554–7565 (2023). https://doi.org/10.1007/s11664-023-10670-w

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