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

Abstract:

:Despite the widespread use of silicon in modern technology, its peculiar thermal expansion is not well understood. Adapting harmonic phonons to the specific volume at temperature, the quasiharmonic approximation, has become accepted for simulating the thermal expansion, but has given ambiguous interpretations for microscopic mechanisms. To test atomistic mechanisms, we performed inelastic neutron scattering experiments from 100 K to 1,500 K on a single crystal of silicon to measure the changes in phonon frequencies. Our state-of-the-art ab initio calculations, which fully account for phonon anharmonicity and nuclear quantum effects, reproduced the measured shifts of individual phonons with temperature, whereas quasiharmonic shifts were mostly of the wrong sign. Surprisingly, the accepted quasiharmonic model was found to predict the thermal expansion owing to a large cancellation of contributions from individual phonons.

authors

Kim DS,Hellman O,Herriman J,Smith HL,Lin JYY,Shulumba N,Niedziela JL,Li CW,Abernathy DL,Fultz B

doi

10.1073/pnas.1707745115

subject

Has Abstract

pub_date

2018-02-27 00:00:00

pages

1992-1997

issue

9

eissn

0027-8424

issn

1091-6490

pii

1707745115

journal_volume

115

pub_type

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