We consider a steady-state(but transient)situation in which a warm dense aggregate is a two-temperature system with equilibrium electrons at temperature T_(e),ions at T_(i),and T_(e)≠T_(i).Such states are achievable ...We consider a steady-state(but transient)situation in which a warm dense aggregate is a two-temperature system with equilibrium electrons at temperature T_(e),ions at T_(i),and T_(e)≠T_(i).Such states are achievable by pump–probe experiments.For warm dense hydrogen in such a twotemperature situation,we investigate nuclear quantum effects(NQEs)on structure and thermodynamic properties,thereby delineating the limitations of ordinary ab initio molecular dynamics.We use path integral molecular dynamics(PIMD)simulations driven by orbital-free density functional theory(OFDFT)calculations with state-of-the-art noninteracting free-energy and exchange-correlation functionals for the explicit temperature dependence.We calibrate the OFDFT calculations against conventional(explicit orbitals)Kohn–Sham DFT.We find that when the ratio of the ionic thermal de Broglie wavelength to the mean interionic distance is larger than about 0.30,the ionic radial distribution function is meaningfully affected by the inclusion of NQEs.Moreover,NQEs induce a substantial increase in both the ionic and electronic pressures.This confirms the importance of NQEs for highly accurate equation-of-state data on highly driven hydrogen.For Te>20 kK,increasing Te in the warm dense hydrogen has slight effects on the ionic radial distribution function and equation of state in the range of densities considered.In addition,we confirm that compared with thermostatted ring-polymer molecular dynamics,the primitive PIMD algorithm overestimates electronic pressures,a consequence of the overly localized ionic description from the primitive scheme.展开更多
基金The majority of this work was done while D.K.was a visitor at the University of Florida.He was supported by the Science Challenge Project of China under Grant No.TZ2016001the NSFC under Grant No.11874424+3 种基金the National Key R&D Program of China under Grant No.2017YFA0403200He also acknowledges support by the China Scholarship Council.K.L.(for the majority of the work done while at the University of Florida)S.B.T.were supported by U.S.Department of Energy Grant No.DE-SC0002139Most of the computations were performed on the HiPerGator-II system at the University of Florida.
文摘We consider a steady-state(but transient)situation in which a warm dense aggregate is a two-temperature system with equilibrium electrons at temperature T_(e),ions at T_(i),and T_(e)≠T_(i).Such states are achievable by pump–probe experiments.For warm dense hydrogen in such a twotemperature situation,we investigate nuclear quantum effects(NQEs)on structure and thermodynamic properties,thereby delineating the limitations of ordinary ab initio molecular dynamics.We use path integral molecular dynamics(PIMD)simulations driven by orbital-free density functional theory(OFDFT)calculations with state-of-the-art noninteracting free-energy and exchange-correlation functionals for the explicit temperature dependence.We calibrate the OFDFT calculations against conventional(explicit orbitals)Kohn–Sham DFT.We find that when the ratio of the ionic thermal de Broglie wavelength to the mean interionic distance is larger than about 0.30,the ionic radial distribution function is meaningfully affected by the inclusion of NQEs.Moreover,NQEs induce a substantial increase in both the ionic and electronic pressures.This confirms the importance of NQEs for highly accurate equation-of-state data on highly driven hydrogen.For Te>20 kK,increasing Te in the warm dense hydrogen has slight effects on the ionic radial distribution function and equation of state in the range of densities considered.In addition,we confirm that compared with thermostatted ring-polymer molecular dynamics,the primitive PIMD algorithm overestimates electronic pressures,a consequence of the overly localized ionic description from the primitive scheme.
