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Title: Phonons in Si 24 at simultaneously elevated temperature and pressure

Abstract

Raman spectroscopy was used to measure the frequencies of phonons in Si 24 with an open clathrate structure at temperatures ranging from 80 to 400 K with simultaneous pressures of 0 to 8 GPa. The frequency shifts of the different phonons were substantially different under either temperature or pressure. The quasiharmonic behavior was isolated by varying pressure at low temperatures, and the anharmonic behavior was isolated by varying temperature at low pressures. Phonon modes dominated by bond bending were anomalous, showing stiffening with temperature and softening with pressure. Both the quasiharmonic behavior and the anharmonic behavior changed markedly with simultaneous changes in temperature Δ T and pressure Δ P . With Δ T = 320 K and Δ P = 8 GPa , some frequency shifts that scaled with the product Δ T Δ P were as large as the shifts from Δ T and Δ P alone. The thermodynamic entropy of this material likely has a dependence on Δ T and Δ P that cannot be obtained by adding effects from quasiharmonicity and phonon-phonon anharmonicity.

Authors:
 [1];  [1];  [1];  [2];  [2];  [3]
  1. California Inst. of Technology (CalTech), Pasadena, CA (United States)
  2. Carnegie Inst. of Washington, Washington, DC (United States)
  3. Carnegie Inst. of Washington, Washington, DC (United States); Center for High Pressure Sciecne and Technology Advanced Research (HPSTAR), Shanghai (China)
Publication Date:
Research Org.:
Energy Frontier Research Centers (EFRC) (United States). Energy Frontier Research in Extreme Environments (EFree)
Sponsoring Org.:
USDOE Office of Science (SC), Basic Energy Sciences (BES)
OSTI Identifier:
1388065
Alternate Identifier(s):
OSTI ID: 1347809
Grant/Contract Number:  
SC0001057
Resource Type:
Accepted Manuscript
Journal Name:
Physical Review B
Additional Journal Information:
Journal Volume: 95; Journal Issue: 9; Related Information: EFree partners with Carnegie Institution of Washington (lead); California Institute of Technology; Colorado School of Mines; Cornell University; Lehigh University; Pennsylvania State University; Journal ID: ISSN 2469-9950
Publisher:
American Physical Society (APS)
Country of Publication:
United States
Language:
English
Subject:
75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND SUPERFLUIDITY; catalysis (heterogeneous), solar (photovoltaic), phonons, thermoelectric, energy storage (including batteries and capacitors), hydrogen and fuel cells, superconductivity, charge transport, mesostructured materials, materials and chemistry by design, synthesis (novel materials)

Citation Formats

Tong, Xiao, Xu, Xiaolin, Fultz, B., Zhang, Haidong, Strobel, Timothy A., and Kim, Duck Young. Phonons in Si24 at simultaneously elevated temperature and pressure. United States: N. p., 2017. Web. doi:10.1103/PhysRevB.95.094306.
Tong, Xiao, Xu, Xiaolin, Fultz, B., Zhang, Haidong, Strobel, Timothy A., & Kim, Duck Young. Phonons in Si24 at simultaneously elevated temperature and pressure. United States. doi:10.1103/PhysRevB.95.094306.
Tong, Xiao, Xu, Xiaolin, Fultz, B., Zhang, Haidong, Strobel, Timothy A., and Kim, Duck Young. Mon . "Phonons in Si24 at simultaneously elevated temperature and pressure". United States. doi:10.1103/PhysRevB.95.094306. https://www.osti.gov/servlets/purl/1388065.
@article{osti_1388065,
title = {Phonons in Si24 at simultaneously elevated temperature and pressure},
author = {Tong, Xiao and Xu, Xiaolin and Fultz, B. and Zhang, Haidong and Strobel, Timothy A. and Kim, Duck Young},
abstractNote = {Raman spectroscopy was used to measure the frequencies of phonons in Si 24 with an open clathrate structure at temperatures ranging from 80 to 400 K with simultaneous pressures of 0 to 8 GPa. The frequency shifts of the different phonons were substantially different under either temperature or pressure. The quasiharmonic behavior was isolated by varying pressure at low temperatures, and the anharmonic behavior was isolated by varying temperature at low pressures. Phonon modes dominated by bond bending were anomalous, showing stiffening with temperature and softening with pressure. Both the quasiharmonic behavior and the anharmonic behavior changed markedly with simultaneous changes in temperature Δ T and pressure Δ P . With Δ T = 320 K and Δ P = 8 GPa , some frequency shifts that scaled with the product Δ T Δ P were as large as the shifts from Δ T and Δ P alone. The thermodynamic entropy of this material likely has a dependence on Δ T and Δ P that cannot be obtained by adding effects from quasiharmonicity and phonon-phonon anharmonicity.},
doi = {10.1103/PhysRevB.95.094306},
journal = {Physical Review B},
number = 9,
volume = 95,
place = {United States},
year = {2017},
month = {3}
}

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