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Title: Phonon anharmonicity in silicon from 100 to 1500 K

Abstract

Inelastic neutron scattering was performed on silicon powder to measure the phonon density of states (DOS) from 100 to 1500 K. The mean fractional energy shifts with temperature of the modes were $$\langle$$Δε iiΔT$$\rangle$$=₋0.07, giving a mean isobaric Grüneisen parameter of +6.95±0.67, which is significantly different from the isothermal parameter of +0.98. These large effects are beyond the predictions from quasiharmonic models using density functional theory or experimental data, demonstrating large effects from phonon anharmonicity. At 1500 K the anharmonicity contributes 0.15k B/atom to the vibrational entropy, compared to 0.03k B/atom from quasiharmonicity. Lastly, excellent agreement was found between the entropy from phonon DOS measurements and the reference NIST-JANAF thermodynamic entropy from calorimetric measurements.

Authors:
 [1];  [1];  [2];  [3];  [4];  [1]
  1. California Inst. of Technology (CalTech), Pasadena, CA (United States). Dept. of Applied Physics and Materials Science
  2. Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States). Instrument and Source Division
  3. Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States). Materials Science & Technology Division
  4. Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States). Quantum Condensed Matter Division
Publication Date:
Research Org.:
Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States). Spallation Neutron Source (SNS)
Sponsoring Org.:
USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22)
OSTI Identifier:
1185765
Alternate Identifier(s):
OSTI ID: 1180194
Grant/Contract Number:  
AC05-00OR22725; FG02-03ER46055
Resource Type:
Accepted Manuscript
Journal Name:
Physical Review. B, Condensed Matter and Materials Physics
Additional Journal Information:
Journal Volume: 91; Journal Issue: 1; Journal ID: ISSN 1098-0121
Publisher:
American Physical Society (APS)
Country of Publication:
United States
Language:
English
Subject:
36 MATERIALS SCIENCE

Citation Formats

Kim, D. S., Smith, Hillary L., Niedziela, Jennifer L., Li, Chen W., Abernathy, Douglas L., and Fultz, B. Phonon anharmonicity in silicon from 100 to 1500 K. United States: N. p., 2015. Web. doi:10.1103/PhysRevB.91.014307.
Kim, D. S., Smith, Hillary L., Niedziela, Jennifer L., Li, Chen W., Abernathy, Douglas L., & Fultz, B. Phonon anharmonicity in silicon from 100 to 1500 K. United States. doi:10.1103/PhysRevB.91.014307.
Kim, D. S., Smith, Hillary L., Niedziela, Jennifer L., Li, Chen W., Abernathy, Douglas L., and Fultz, B. Wed . "Phonon anharmonicity in silicon from 100 to 1500 K". United States. doi:10.1103/PhysRevB.91.014307. https://www.osti.gov/servlets/purl/1185765.
@article{osti_1185765,
title = {Phonon anharmonicity in silicon from 100 to 1500 K},
author = {Kim, D. S. and Smith, Hillary L. and Niedziela, Jennifer L. and Li, Chen W. and Abernathy, Douglas L. and Fultz, B.},
abstractNote = {Inelastic neutron scattering was performed on silicon powder to measure the phonon density of states (DOS) from 100 to 1500 K. The mean fractional energy shifts with temperature of the modes were $\langle$Δεi/εiΔT$\rangle$=₋0.07, giving a mean isobaric Grüneisen parameter of +6.95±0.67, which is significantly different from the isothermal parameter of +0.98. These large effects are beyond the predictions from quasiharmonic models using density functional theory or experimental data, demonstrating large effects from phonon anharmonicity. At 1500 K the anharmonicity contributes 0.15kB/atom to the vibrational entropy, compared to 0.03kB/atom from quasiharmonicity. Lastly, excellent agreement was found between the entropy from phonon DOS measurements and the reference NIST-JANAF thermodynamic entropy from calorimetric measurements.},
doi = {10.1103/PhysRevB.91.014307},
journal = {Physical Review. B, Condensed Matter and Materials Physics},
number = 1,
volume = 91,
place = {United States},
year = {2015},
month = {1}
}

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