论文标题

通过不同的实时时间依赖性构型相互作用方法,探索氢分子中的Attosend激光驱动的电子动力学

Exploring the attosecond laser-driven electron dynamics in the hydrogen molecule with different real-time time-dependent configuration interaction approaches

论文作者

Woźniak, Aleksander P., Lewenstein, Maciej, Moszyński, Robert

论文摘要

与高斯基集相连的时间依赖性量子化学方法在建模与强激光场相互作用的原子和分子的电子动力学中越来越流行。两种用于此目的最广泛使用的方法,即实时时间依赖于时间依赖的配置相互作用单和实时依赖时间的密度功能理论,它们都有其局限性,因此开发更准确但计算上有效的时间相关方法仍在需求中。在这项工作中,我们探讨了实时时间相关的配置相互作用单打和双打(RT-TDCISD)在建模强场现象中的适用性。由于RT-TDCISD的主要缺点是其不利的缩放,因此我们通过选择这些应该在波函数的时间进化中具​​有主要贡献的CISD特征状态来开发几种算法来减少有效传播空间。我们通过对H \ TextSubscript {2}分子的高谐波光谱进行计算来测试它们。我们发现,激光驱动的电子动力学主要是在以单个激发为主的非常小的特征状态的子空间中实现的,这占整个CISD特征的百分之一。因此,通过正确选择此子空间,可以将传播方程的维度降低两个数量级,而不会影响时间分辨可观察到。

Time-dependent quantum chemical methods coupled to Gaussian basis sets are gaining popularity in modeling the electron dynamics of atoms and molecules interacting with intense laser fields. Two approaches most widely used for this purpose, the real-time time-dependent configuration interaction singles and the real-time time-dependent density functional theory, both have their limitations, so the development of more accurate yet computationally efficient time-dependent methods is still in demand. In this work we explore the applicability of the real-time time-dependent configuration interaction singles and doubles (RT-TDCISD) in modeling strong field phenomena. Since the main drawback of RT-TDCISD is its unfavourable scaling, we develop several algorithms for reducing the effective propagation space by selecting these CISD eigenstates that should have dominant contribution to the time-evolution of the wavefunction. We test them by performing calculations of the high harmonic spectra of the H\textsubscript{2} molecule. We find out that the laser-driven electron dynamics is mostly realized in a very small subspace of eigenstates dominated by single excitations, that constitutes about one percent of the whole CISD eigenspectrum. Therefore, by properly selecting this subspace one can reduce the dimension of the propagation equation by two orders of magnitude without affecting the time-resolved observables.

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