The high pressure behaviors of Th_4H_（15） and ThH_2 are investigated by using the first-principles calculations based on the density functional theory（DFT）. From the energy–volume relations, the bct phase of ThH_...The high pressure behaviors of Th_4H_（15） and ThH_2 are investigated by using the first-principles calculations based on the density functional theory（DFT）. From the energy–volume relations, the bct phase of ThH_2 is more stable than the fcc phase at ambient conditions. At high pressure, the bct ThH_2 and bcc Th_4H（15） phases are more brittle than they are at ambient pressure from the calculated elastic constants and the Poisson ratio. The thermodynamic stability of the bct phase ThH_2 is determined from the calculated phonon dispersion. In the pressure domain of interest, the phonon dispersions of bcc Th_4H（15） and bct ThH_2 are positive, indicating the dynamical stability of these two phases, while the fcc ThH_2 is unstable. The thermodynamic properties including the lattice vibration energy, entropy, and specific heat are predicted for these stable phases. The vibrational free energy decreases with the increase of the temperature, and the entropy and the heat capacity are proportional to the temperature and inversely proportional to the pressure. As the pressure increases, the resistance to the external pressure is strengthened for Th_4H_（15） and ThH_2.展开更多
基金Project supported by the Long-Term Subsidy Mechanism from the Ministry of Finance and the Ministry of Education of China
文摘The high pressure behaviors of Th_4H_（15） and ThH_2 are investigated by using the first-principles calculations based on the density functional theory（DFT）. From the energy–volume relations, the bct phase of ThH_2 is more stable than the fcc phase at ambient conditions. At high pressure, the bct ThH_2 and bcc Th_4H（15） phases are more brittle than they are at ambient pressure from the calculated elastic constants and the Poisson ratio. The thermodynamic stability of the bct phase ThH_2 is determined from the calculated phonon dispersion. In the pressure domain of interest, the phonon dispersions of bcc Th_4H（15） and bct ThH_2 are positive, indicating the dynamical stability of these two phases, while the fcc ThH_2 is unstable. The thermodynamic properties including the lattice vibration energy, entropy, and specific heat are predicted for these stable phases. The vibrational free energy decreases with the increase of the temperature, and the entropy and the heat capacity are proportional to the temperature and inversely proportional to the pressure. As the pressure increases, the resistance to the external pressure is strengthened for Th_4H_（15） and ThH_2.
