We demonstrate high-harmonic spectroscopy in many-electron molecules using time-dependent density-functional theory. We show that a weak attosecond-pulse-train ionization seed that is properly synchronized with the strong driving mid-infrared laser field can produce experimentally relevant high-harmonic generation (HHG) signals, from which we extract both the spectral amplitude and the target-specific phase (group delay). We also show that further processing of the HHG signal can be used to achieve molecular-frame resolution, i.e., to resolve the contributions from rescattering on different sides of an oriented molecule. In this framework, we investigate transient two-center interference in CO2 and OCS, and how subcycle polarization effects shape the oriented/aligned angle-resolved spectra.

中文翻译：

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利用瞬态二中心干涉的高次谐波谱计算的瞬态密度泛函理论。


我们使用时间相关的密度泛函理论演示了多电子分子的高次谐波光谱。我们证明，与强驱动中红外激光场正确同步的弱阿秒脉冲序列电离种子可以产生实验相关的高次谐波发生（HHG）信号，我们从中提取光谱幅度和目标-特定相位（群延迟）。我们还表明，对 HHG 信号的进一步处理可用于实现分子框架分辨率，即解决定向分子不同侧面上的重新散射的贡献。在此框架中，我们研究了 CO2 和 OCS 中的瞬态双中心干涉，以及亚周期偏振效应如何塑造定向/对齐的角度分辨光谱。