Livshits Ester, Baer Roi
Department of Physical Chemistry and the Lise Meitner Minerva-Center for Quantum Chemistry, Hebrew University of Jerusalem, Jerusalem 91904, Israel.
J Phys Chem A. 2006 Jul 13;110(27):8443-50. doi: 10.1021/jp0600460.
Real-time first principle simulations are presented of the D(2) Coulomb explosion dynamics detonated by exposure to very intense few-cycle laser pulse. Three approximate functionals within the time-dependent density functional theory (TDDFT) functionals are examined for describing the electron dynamics, including time-dependent Hartree-Fock theory. Nuclei are treated classically with quantum corrections. The calculated results are sensitive to the underlying electronic structure theory, showing too narrow kinetic energy distribution peaked at too high kinetic energy when compared with recent experimental results (Phys. Rev. Lett. 2003, 91, 093002). Experiment also shows a low energy peak which is not seen in the present calculation. We conclude that while Ehrenfest-adiabatic-TDDFT can qualitatively account for the dynamics, it requires further development, probably beyond the adiabatic approximation, to be quantitative.
本文展示了通过暴露于极短周期超强激光脉冲引发的D(2)库仑爆炸动力学的实时第一性原理模拟。研究了含时密度泛函理论（TDDFT）中的三种近似泛函来描述电子动力学，包括含时哈特里-福克理论。原子核采用经典处理并考虑量子修正。计算结果对基础电子结构理论很敏感，与近期实验结果（《物理评论快报》2003年，91卷，093002期）相比，其动能分布过窄且峰值动能过高。实验还显示出一个在当前计算中未出现的低能峰。我们得出结论，虽然埃伦费斯特绝热含时密度泛函理论能定性地解释动力学，但要实现定量描述，可能需要进一步发展，或许要超越绝热近似。
