Equation of state, phase transitions, and band-gap closure in Pb Cl 2 and Sn Cl 2
Abstract
The equations of state and band-gap closures for Pb Cl2 and Sn Cl2 were studied using both experimental and theoretical methods. Here we measured the volume of both materials to a maximum pressure of 70 GPa using synchrotron-based angle-dispersive powder x-ray diffraction. The lattice parameters for both compounds showed anomalous changes between 16–32 GPa, providing evidence of a phase transition from the cotunnite structure to the related Co2 Si structure, in contrast to the postcotunnite structure as previously suggested. First-principles calculations confirm this finding and predict a second phase transition to a Co2 Si-like structure between 75– 110 GPa in Pb Cl2 and 60–75 GPa in Sn Cl2. Band gaps were measured under compression to ~70 GPa for Pb Cl2 and ~66 GPa for Sn Cl2 and calculated up to 200 GPa for Pb CI2 and 120 GPa for Sn Cl2. We find an excellent agreement between our experimental and theoretical results when using the Heyd-Scuseria-Ernzerhof (HSE06) hybrid functional, which suggests that this functional could reliably be used to calculate the band gap of similar AX2 compounds. Experimental and calculated band-gap results show discontinuous decreases in the band gap corresponding to phase changes to higher-coordinated crystal structures, giving insight intomore »
- Authors:
-
- Univ. of California, Berkeley, CA (United States)
- Lawrence Livermore National Lab. (LLNL), Livermore, CA (United States)
- University of Leeds (United Kingdom)
- Univ. of California, Santa Cruz, CA (United States)
- Publication Date:
- Research Org.:
- Lawrence Livermore National Laboratory (LLNL), Livermore, CA (United States); Lawrence Berkeley National Laboratory (LBNL), Berkeley, CA (United States). Advanced Light Source (ALS)
- Sponsoring Org.:
- USDOE National Nuclear Security Administration (NNSA); National Science Foundation (NSF); USDOE Office of Science (SC), Basic Energy Sciences (BES); Natural Environment Research Council (NERC)
- OSTI Identifier:
- 1972037
- Report Number(s):
- LLNL-JRNL-815142
Journal ID: ISSN 2469-9950; 1023161; TRN: US2313748
- Grant/Contract Number:
- AC52-07NA27344; NA0004032; AC02-05CH11231; EAR-1620423; EAR 16–06856; NE/K006290/1
- Resource Type:
- Accepted Manuscript
- Journal Name:
- Physical Review. B
- Additional Journal Information:
- Journal Volume: 107; Journal Issue: 13; Journal ID: ISSN 2469-9950
- Publisher:
- American Physical Society (APS)
- Country of Publication:
- United States
- Language:
- English
- Subject:
- 36 MATERIALS SCIENCE; 75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND SUPERFLUIDITY; high-pressure studies; metal-insulator transition; density functional theory; x-ray powder diffraction; AX2 compounds; SnCI2; metallization
Citation Formats
Smart, T. J., O’Bannon, E. F., Diamond, M. R., Stackhouse, S., Godwal, B. K., Williams, Q., and Jeanloz, R. Equation of state, phase transitions, and band-gap closure in PbCl2 and SnCl2. United States: N. p., 2023.
Web. doi:10.1103/physrevb.107.134113.
Smart, T. J., O’Bannon, E. F., Diamond, M. R., Stackhouse, S., Godwal, B. K., Williams, Q., & Jeanloz, R. Equation of state, phase transitions, and band-gap closure in PbCl2 and SnCl2. United States. https://doi.org/10.1103/physrevb.107.134113
Smart, T. J., O’Bannon, E. F., Diamond, M. R., Stackhouse, S., Godwal, B. K., Williams, Q., and Jeanloz, R. Thu .
"Equation of state, phase transitions, and band-gap closure in PbCl2 and SnCl2". United States. https://doi.org/10.1103/physrevb.107.134113. https://www.osti.gov/servlets/purl/1972037.
@article{osti_1972037,
title = {Equation of state, phase transitions, and band-gap closure in PbCl2 and SnCl2},
author = {Smart, T. J. and O’Bannon, E. F. and Diamond, M. R. and Stackhouse, S. and Godwal, B. K. and Williams, Q. and Jeanloz, R.},
abstractNote = {The equations of state and band-gap closures for Pb Cl2 and Sn Cl2 were studied using both experimental and theoretical methods. Here we measured the volume of both materials to a maximum pressure of 70 GPa using synchrotron-based angle-dispersive powder x-ray diffraction. The lattice parameters for both compounds showed anomalous changes between 16–32 GPa, providing evidence of a phase transition from the cotunnite structure to the related Co2 Si structure, in contrast to the postcotunnite structure as previously suggested. First-principles calculations confirm this finding and predict a second phase transition to a Co2 Si-like structure between 75– 110 GPa in Pb Cl2 and 60–75 GPa in Sn Cl2. Band gaps were measured under compression to ~70 GPa for Pb Cl2 and ~66 GPa for Sn Cl2 and calculated up to 200 GPa for Pb CI2 and 120 GPa for Sn Cl2. We find an excellent agreement between our experimental and theoretical results when using the Heyd-Scuseria-Ernzerhof (HSE06) hybrid functional, which suggests that this functional could reliably be used to calculate the band gap of similar AX2 compounds. Experimental and calculated band-gap results show discontinuous decreases in the band gap corresponding to phase changes to higher-coordinated crystal structures, giving insight into the relationship between interatomic geometry and metallicity.},
doi = {10.1103/physrevb.107.134113},
journal = {Physical Review. B},
number = 13,
volume = 107,
place = {United States},
year = {Thu Apr 20 00:00:00 EDT 2023},
month = {Thu Apr 20 00:00:00 EDT 2023}
}
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