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Title: Synthesis of a mixed-valent tin nitride and considerations of its possible crystal structures

Abstract

Recent advances in theoretical structure prediction methods and high-throughput computational techniques are revolutionizing experimental discovery of the thermodynamically stable inorganic materials. Metastable materials represent a new frontier for these studies, since even simple binary non-ground state compounds of common elements may be awaiting discovery. However, there are significant research challenges related to non-equilibrium thin film synthesis and crystal structure predictions, such as small strained crystals in the experimental samples and energy minimization based theoretical algorithms. Here, we report on experimental synthesis and characterization, as well as theoretical first-principles calculations of a previously unreported mixed-valent binary tin nitride. Thin film experiments indicate that this novel material is N-deficient SnN with tin in the mixed ii/iv valence state and a small low-symmetry unit cell. Theoretical calculations suggest that the most likely crystal structure has the space group 2 (SG2) related to the distorted delafossite (SG166), which is nearly 0.1 eV/atom above the ground state SnN polymorph. This observation is rationalized by the structural similarity of the SnN distorted delafossite to the chemically related Sn 3 N 4 spinel compound, which provides a fresh scientific insight into the reasons for growth of polymorphs of metastable materials. In addition to reporting on the discoverymore » of the simple binary SnN compound, this paper illustrates a possible way of combining a wide range of advanced characterization techniques with the first-principle property calculation methods, to elucidate the most likely crystal structure of the previously unreported metastable materials.« less

Authors:
 [1];  [2];  [3];  [2];  [3];  [4];  [2];  [4];  [5];  [5];  [6];  [7];  [6];  [8];  [9];  [2];  [2];  [2];  [10];  [3] more »;  [2];  [3];  [2] « less
  1. National Renewable Energy Lab. (NREL), Golden, CO (United States); Colorado School of Mines, Golden, CO (United States); Larix Chemical Sciences, Golden, CO (United States)
  2. National Renewable Energy Lab. (NREL), Golden, CO (United States)
  3. Colorado School of Mines, Golden, CO (United States)
  4. SLAC National Accelerator Lab., Menlo Park, CA (United States)
  5. Tel Aviv Univ., Ramat Aviv (Israel)
  6. Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States)
  7. Massachusetts Inst. of Technology (MIT), Cambridge, MA (United States)
  8. Univ. of Colorado, Boulder, CO (United States)
  9. Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States); Massachusetts Inst. of Technology (MIT), Cambridge, MA (United States)
  10. National Renewable Energy Lab. (NREL), Golden, CO (United States); Colorado School of Mines, Golden, CO (United States)
Publication Date:
Research Org.:
Energy Frontier Research Centers (EFRC) (United States). Center for Next Generation of Materials by Design: Incorporating Metastability (CNGMD); National Renewable Energy Lab. (NREL), Golden, CO (United States); SLAC National Accelerator Lab., Menlo Park, CA (United States); Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States)
Sponsoring Org.:
USDOE Office of Science (SC), Basic Energy Sciences (BES); National Institutes of Health (NIH); Univ. of California, Los Angeles, CA (United States). California NanoSystems Inst. (CNSI); National Science Foundation (NSF)
OSTI Identifier:
1248078
Alternate Identifier(s):
OSTI ID: 1247018; OSTI ID: 1257738; OSTI ID: 1440926
Report Number(s):
NREL/JA-5K00-66167; SLAC-PUB-16560
Journal ID: ISSN 0021-9606
Grant/Contract Number:  
AC36-08GO28308; AC02-76SF00515; AC36-99GO10337; AC02-05CH11231; CMMI-1200547; DEAC36-08GO28308
Resource Type:
Accepted Manuscript
Journal Name:
Journal of Chemical Physics
Additional Journal Information:
Journal Volume: 144; Journal Issue: 14; Related Information: Journal of Chemical Physics; Journal ID: ISSN 0021-9606
Publisher:
American Institute of Physics (AIP)
Country of Publication:
United States
Language:
English
Subject:
37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY; 36 MATERIALS SCIENCE; crystal structure; x-ray diffraction; tin; polymorphism; x-ray absorption spectroscopy

Citation Formats

Caskey, Christopher M., Holder, Aaron, Shulda, Sarah, Christensen, Steven T., Diercks, David, Schwartz, Craig P., Biagioni, David, Nordlund, Dennis, Kukliansky, Alon, Natan, Amir, Prendergast, David, Orvananos, Bernardo, Sun, Wenhao, Zhang, Xiuwen, Ceder, Gerbrand, Ginley, David S., Tumas, William, Perkins, John D., Stevanovic, Vladan, Pylypenko, Svitlana, Lany, Stephan, Richards, Ryan M., and Zakutayev, Andriy. Synthesis of a mixed-valent tin nitride and considerations of its possible crystal structures. United States: N. p., 2016. Web. doi:10.1063/1.4945561.
Caskey, Christopher M., Holder, Aaron, Shulda, Sarah, Christensen, Steven T., Diercks, David, Schwartz, Craig P., Biagioni, David, Nordlund, Dennis, Kukliansky, Alon, Natan, Amir, Prendergast, David, Orvananos, Bernardo, Sun, Wenhao, Zhang, Xiuwen, Ceder, Gerbrand, Ginley, David S., Tumas, William, Perkins, John D., Stevanovic, Vladan, Pylypenko, Svitlana, Lany, Stephan, Richards, Ryan M., & Zakutayev, Andriy. Synthesis of a mixed-valent tin nitride and considerations of its possible crystal structures. United States. doi:10.1063/1.4945561.
Caskey, Christopher M., Holder, Aaron, Shulda, Sarah, Christensen, Steven T., Diercks, David, Schwartz, Craig P., Biagioni, David, Nordlund, Dennis, Kukliansky, Alon, Natan, Amir, Prendergast, David, Orvananos, Bernardo, Sun, Wenhao, Zhang, Xiuwen, Ceder, Gerbrand, Ginley, David S., Tumas, William, Perkins, John D., Stevanovic, Vladan, Pylypenko, Svitlana, Lany, Stephan, Richards, Ryan M., and Zakutayev, Andriy. Tue . "Synthesis of a mixed-valent tin nitride and considerations of its possible crystal structures". United States. doi:10.1063/1.4945561. https://www.osti.gov/servlets/purl/1248078.
@article{osti_1248078,
title = {Synthesis of a mixed-valent tin nitride and considerations of its possible crystal structures},
author = {Caskey, Christopher M. and Holder, Aaron and Shulda, Sarah and Christensen, Steven T. and Diercks, David and Schwartz, Craig P. and Biagioni, David and Nordlund, Dennis and Kukliansky, Alon and Natan, Amir and Prendergast, David and Orvananos, Bernardo and Sun, Wenhao and Zhang, Xiuwen and Ceder, Gerbrand and Ginley, David S. and Tumas, William and Perkins, John D. and Stevanovic, Vladan and Pylypenko, Svitlana and Lany, Stephan and Richards, Ryan M. and Zakutayev, Andriy},
abstractNote = {Recent advances in theoretical structure prediction methods and high-throughput computational techniques are revolutionizing experimental discovery of the thermodynamically stable inorganic materials. Metastable materials represent a new frontier for these studies, since even simple binary non-ground state compounds of common elements may be awaiting discovery. However, there are significant research challenges related to non-equilibrium thin film synthesis and crystal structure predictions, such as small strained crystals in the experimental samples and energy minimization based theoretical algorithms. Here, we report on experimental synthesis and characterization, as well as theoretical first-principles calculations of a previously unreported mixed-valent binary tin nitride. Thin film experiments indicate that this novel material is N-deficient SnN with tin in the mixed ii/iv valence state and a small low-symmetry unit cell. Theoretical calculations suggest that the most likely crystal structure has the space group 2 (SG2) related to the distorted delafossite (SG166), which is nearly 0.1 eV/atom above the ground state SnN polymorph. This observation is rationalized by the structural similarity of the SnN distorted delafossite to the chemically related Sn 3 N 4 spinel compound, which provides a fresh scientific insight into the reasons for growth of polymorphs of metastable materials. In addition to reporting on the discovery of the simple binary SnN compound, this paper illustrates a possible way of combining a wide range of advanced characterization techniques with the first-principle property calculation methods, to elucidate the most likely crystal structure of the previously unreported metastable materials.},
doi = {10.1063/1.4945561},
journal = {Journal of Chemical Physics},
number = 14,
volume = 144,
place = {United States},
year = {2016},
month = {4}
}

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