@article{68b9735fc8c64daf91eceb66afffe2aa,
title = "Antimony nitride discovered by theoretical structure prediction, rapid thermal annealing, and in situ X-ray diffraction",
abstract = "Nitride materials have promising properties for optoelectronics, but synthesis is challenging because of their metastable character. Therefore, even some simple binary nitrides have not been reported, and their properties remain unknown. Here, we report a metastable Sb–N phase. Unconstrained first-principle crystal-structure predictions suggest that a semiconducting layered SbN phase could be synthesized under activated nitrogen conditions. Experimentally, we approach the synthesis by rapid thermal annealing of an amorphous thin-film precursor. In situ X-ray diffraction monitoring reveals a transient phase appearing at 500°C and lasting for 17 s. With molecular dynamics simulations, we conclude that the phase observed is related to the predicted ground-state structure but that it contains stacking variations. This research highlights the synergy between computational materials discovery and in situ structural characterization during synthesis and processing, enabling the identification and synthesizability of new materials at the frontier of thermodynamically metastable regions.",
keywords = "first-principle calculations, in situ X-ray scatting, metastable, nitride materials, rapid thermal annealing, sputtering",
author = "Chen, \{Bor Rong\} and Stephan Lany and Kelly, \{Leah L.\} and Elisabetta Arca and Yuki Iguchi and Perkins, \{John D.\} and Hiroshi Yanagi and Toney, \{Michael F.\} and Schelhas, \{Laura T.\} and Andriy Zakutayev",
note = "Funding Information: This work was authored at the National Renewable Energy Laboratory, operated by Alliance for Sustainable Energy, LLC, for the US Department of Energy (DOE) under contract no. DE-AC36-08GO28308. Funding was provided by the Office of Science, Basic Energy Sciences, Materials Sciences and Engineering (MSE) Division; as a part of Energy Frontier Research Center's “Center for Next Generation Materials by Design: Incorporating Metastability” (computational predictions and in situ measurements); and as a part of Materials Chemistry Program Early Career Award “Kinetic Synthesis of Metastable Nitrides” (materials synthesis and characterization). Use of the Stanford Synchrotron Radiation Light Source, SLAC National Accelerator Laboratory, was supported by the US DOE, Office of Basic Energy Sciences under contract no. DE-AC02-76SF00515. The authors would like to thank Douglas Van Campen for building the in situ RTA chamber and Bart Johnson for beamline support at BL 7-2. High-performance computing resources were sponsored by the DOE and the Office of Energy Efficiency and Renewable Energy. The views expressed in the article do not necessarily represent the views of the DOE or the US government. A.Z. S.L. M.F.T. and L.T.S. originated the research. S.L. performed first-principle theoretical predictions. Y.I. and E.A. prepared Sb–N thin-film samples, and Y.I. and H.Y. performed and analyzed RTA and ex situ XRD experiments. J.D.P. measured and analyzed composition by RBS. L.T.S. performed in situ XRD experiments, and B.-R.C. L.L.K. M.F.T. and L.T.S. analyzed the in situ diffraction data. The manuscript was primarily written by B.-R.C. S.L. L.L.K. and A.Z. All authors contributed to discussions and manuscript review. The authors declare no competing interests. Funding Information: This work was authored at the National Renewable Energy Laboratory, operated by Alliance for Sustainable Energy, LLC, for the US Department of Energy (DOE) under contract no. DE-AC36-08GO28308 . Funding was provided by the Office of Science , Basic Energy Sciences , Materials Sciences and Engineering (MSE) Division; as a part of Energy Frontier Research Center{\textquoteright}s “Center for Next Generation Materials by Design: Incorporating Metastability” (computational predictions and in situ measurements); and as a part of Materials Chemistry Program Early Career Award “Kinetic Synthesis of Metastable Nitrides” (materials synthesis and characterization). Use of the Stanford Synchrotron Radiation Light Source, SLAC National Accelerator Laboratory, was supported by the US DOE , Office of Basic Energy Sciences under contract no. DE-AC02-76SF00515 . The authors would like to thank Douglas Van Campen for building the in situ RTA chamber and Bart Johnson for beamline support at BL 7-2. High-performance computing resources were sponsored by the DOE and the Office of Energy Efficiency and Renewable Energy. The views expressed in the article do not necessarily represent the views of the DOE or the US government. Publisher Copyright: {\textcopyright} 2022 The Authors",
year = "2022",
month = aug,
day = "17",
doi = "10.1016/j.xcrp.2022.100980",
language = "English",
volume = "3",
journal = "Cell Reports Physical Science",
issn = "2666-3864",
publisher = "Cell Press",
number = "8",
}