Phonon anharmonicity and components of the entropy in palladium and platinum

Article

关键词: TOTAL-ENERGY CALCULATIONS;    WAVE BASIS-SET;    THERMODYNAMIC PROPERTIES;    SINGLE-CRYSTALS;    PRESSURE SCALES;    METALS;    TEMPERATURES;    SCATTERING;    DYNAMICS;    STATE;   

DOI  :  10.1103/PhysRevB.93.214303

来源: SCIE

【 摘 要 】

Inelastic neutron scattering was used to measure the phonon density of states in fcc palladium and platinum metal at temperatures from 7 K to 1576 K. Both phonon-phonon interactions and electron-phonon interactions were calculated by methods based on density functional theory (DFT) and were consistent with the measured shifts and broadenings of phonons with temperature. Unlike the longitudinal modes, the characteristic transverse modes had a nonlinear dependence on temperature owing to the requirement for a population of thermal phonons for upscattering. Kohn anomalies were observed in the measurements at low temperature and were reproduced by calculations based on DFT. Contributions to the entropy from phonons and electrons were assessed and summed to obtain excellent agreement with prior calorimetric data. The entropy from thermal expansion is positive for both phonons and electrons but larger for phonons. The anharmonic phonon entropy is negative in Pt, but in Pd it changes from positive to negative with increasing temperature. Owing to the position of the Fermi level on the electronic DOS, the electronic entropy was sensitive to the adiabatic electron-phonon interaction in both Pd and Pt. The adiabatic EPI depended strongly on thermal atom displacements.

【 授权许可】

Free