We present a theoretical investigation as to how multielectron dynamics of CO are manipulated by Fourier-synthesized intense laser pulses. The pulses used are assumed to be comprised of harmonics up to the fourth order. The multiconfiguration time-dependent (TD) Hartree-Fock (MCTDHF) method, where the multielectron wavefunction is expressed as a linear combination of various electron configurations, is employed to simulate the dynamics of CO interacting with Fourier-synthesized pulses. The multielectron nature such as electron correlation is quantified by using our effective potential approach. To begin with, the time-dependent natural orbitals which diagonalize the first order reduced density matrix are obtained from the MCTDHF wave function. The effective potentials that determine the dynamics of natural orbitals are then derived, which consists of the one-body part including the interaction with the laser electric field and the two-body part originating from electron-electron interaction. The role of electron correlation can be quantified by comparing the effective potentials obtained with those obtained by the TDHF method. We found a very similar profile in the effective potential of the 5sigma highest occupied molecular orbital (HOMO) for one-color (omega) and directionally asymmetric omega +2omega two-color pulses; when the electric field points from C to O, a hump (or shoulder) appears in the effective potential only 2 bohrs outward from C. The hump formation, which originates from the field-induced change in the two-body part (especially, due to electron correlation), is responsible for experimentally observed anisotropic ionization from the C atom side. A coherent superposition of omega and 2omega fields with an appropriate relative phase works as a one-color pulse of which either positive or negative peaks are filtered out. More sophisticated manipulation is possible by adding higher harmonics to a synthesized field. We show that the 5sigma orbital can be squeezed toward the inside of the valley in the effective potential, which encloses the molecule at a radius of ~7 bohrs (semicircle in the region of z <0), by adjusting the phases of a four-color field. We found that hump and valley formation in the effective potential are closely correlated with domains of increasing and decreasing electron density, respectively.

中文翻译：

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通过傅里叶合成强激光脉冲操纵分子的多电子动力学：CO 的有效电位分析

我们对傅立叶合成的强激光脉冲如何操纵 CO 的多电子动力学进行了理论研究。假设使用的脉冲由高达四阶的谐波组成。多配置时间相关 (TD) Hartree-Fock (MCTDHF) 方法，其中多电子波函数表示为各种电子配置的线性组合，用于模拟 CO 与傅立叶合成脉冲相互作用的动力学。通过使用我们的有效电位方法可以量化多电子性质，例如电子相关性。首先，从 MCTDHF 波函数中获得对角化一阶约化密度矩阵的时间相关自然轨道。然后得出确定自然轨道动力学的有效势，它由包括与激光电场相互作用的一体部分和源自电子-电子相互作用的二部分组成。电子相关性的作用可以通过将获得的有效电位与通过 TDHF 方法获得的有效电位进行比较来量化。我们发现单色 (omega) 和方向不对称 omega +2omega 双色脉冲的 5sigma 最高占据分子轨道 (HOMO) 的有效电位非常相似；当电场从 C 指向 O 时，在距离 C 仅 2 bohrs 的有效电位中出现一个驼峰（或肩部）。 驼峰的形成源于两体部分的场致变化（特别是由于到电子相关），负责从 C 原子侧实验观察到的各向异性电离。具有适当相对相位的 omega 和 2omega 场的相干叠加用作单色脉冲，其中正峰值或负峰值被滤除。通过向合成场添加高次谐波，可以进行更复杂的操作。我们表明 5sigma 轨道可以被挤压到有效势谷的内部，通过调整四相的相位，有效势将分子包围在半径约 7 玻尔（z < 0 区域的半圆）处。色域。我们发现有效电位中的驼峰和谷形成分别与电子密度的增加和减少域密切相关。通过向合成场添加高次谐波，可以进行更复杂的操作。我们表明 5sigma 轨道可以被挤压到有效势谷的内部，通过调整四相的相位，有效势将分子包围在半径约 7 玻尔（z < 0 区域的半圆）处。色域。我们发现有效电位中的驼峰和谷形成分别与电子密度的增加和减少域密切相关。通过向合成场中添加更高的谐波，可以进行更复杂的操作。我们表明 5sigma 轨道可以被挤压到有效势谷的内部，通过调整四相的相位，有效势将分子包围在半径约 7 玻尔（z < 0 区域的半圆）处。色域。我们发现有效电位中的驼峰和谷形成分别与电子密度的增加和减少域密切相关。