Origin of the transition entropy in vanadium dioxide

Article

关键词: METAL-INSULATOR-TRANSITION;    TOTAL-ENERGY CALCULATIONS;    CRYSTAL STABILITY;    VO2;    OXIDE;   

DOI  :  10.1103/PhysRevB.99.064113

来源: SCIE

【 摘 要 】

The reversible metal-insulator transition in VO2 at T-c approximate to 340 K has been closely scrutinized yet its thermodynamic origin remains ambiguous. We discuss the origin of the transition entropy by calculating the electron and phonon contributions at T-c using density functional theory. The vibration frequencies are obtained from harmonic phonon calculations, with the soft modes that are imaginary at zero temperature renormalized to real values at T-c using experimental information from diffuse x-ray scattering at high-symmetry wave vectors. Gaussian process regression is used to infer the transformed frequencies for wave vectors across the whole Brillouin zone, and in turn compute the finite temperature phonon partition function to predict transition thermodynamics. Using this method, we predict the phase transition in VO2 is driven 5 to 1 by phonon entropy over electronic entropy, and predict a total transition entropy that agrees (within 5%) with the calorimetric value.

【 授权许可】

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