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Title: Nuclear quantum effect with pure anharmonicity and the anomalous thermal expansion of silicon

Journal Article · · Proceedings of the National Academy of Sciences of the United States of America
ORCiD logo [1];  [1];  [1];  [1]; ORCiD logo [2];  [3];  [4];  [5];  [6];  [1]
  1. Department of Applied Physics and Materials Science, California Institute of Technology, Pasadena, CA 91125,
  2. Neutron Data Analysis and Visualization Division, Oak Ridge National Laboratory, Oak Ridge, TN 37831,
  3. Department of Mechanical and Civil Engineering, California Institute of Technology, Pasadena, CA 91125,
  4. Instrument and Source Division, Oak Ridge National Laboratory, Oak Ridge, TN 37831,
  5. Department of Mechanical Engineering, University of California, Riverside, CA 92521,
  6. Quantum Condensed Matter Division, Oak Ridge National Laboratory, Oak Ridge, TN 37831
+ Show Author Affiliations

Significance Silicon has a peculiar negative thermal expansion at low temperature. This behavior has been understood with a “quasiharmonic” theory where low-energy phonons decrease in frequency with volume contraction. We report inelastic neutron scattering measurements of phonon dispersions over a wide range of temperatures. These measurements cast doubt upon quasiharmonic theory, which predicts the wrong sign for most phonon shifts with temperature. Fully anharmonic ab initio calculations correctly predict the phonon shifts and thermal expansion. Crystal structure, anharmonicity, and nuclear quantum effects all play important roles in the thermal expansion of silicon, and a simple mechanical explanation is inappropriate. The quantum effect of nuclear vibrations is also expected to be important for thermophysical properties of many materials.

Research Organization:
California Inst. of Technology (CalTech), Pasadena, CA (United States); Lawrence Berkeley National Laboratory (LBNL), Berkeley, CA (United States). National Energy Research Scientific Computing Center (NERSC); Univ. of California, Oakland, CA (United States)
Sponsoring Organization:
USDOE Office of Science (SC); USDOE Office of Science (SC), Basic Energy Sciences (BES)
Grant/Contract Number:
AC02-05CH11231; FG02-03ER46055
OSTI ID:
1420356
Journal Information:
Proceedings of the National Academy of Sciences of the United States of America, Journal Name: Proceedings of the National Academy of Sciences of the United States of America Journal Issue: 9 Vol. 115; ISSN 0027-8424
Publisher:
Proceedings of the National Academy of SciencesCopyright Statement
Country of Publication:
United States
Language:
English

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Other Topics
Science & Technology
inelastic neutron scattering
nuclear quantum effects
phonon anharmonicity
silicon
thermal expansion