Abstract This review discusses recent experimental and theoretical analyses of high-harmonic spectroscopy in small molecules, with the aim of characterizing charge migration. We discuss the formulation of molecular high-harmonic spectra followed by methods to extract molecular-target-specific information, both in experiments and ab initio simulations. We present measured and simulated high-harmonic spectra from carbon dioxide and carbonyl sulfide to illustrate the necessity for multidimensional analyses for high-harmonic spectroscopies that include both the spectral amplitude and phase. Leveraging these results, we examine how such multidimensional analyses pave the way for the study of charge migration with high-harmonic spectroscopy and illustrate the beneficial role a static molecular feature can play when probing dynamics. Finally, we briefly expand our scope with an outlook on the critical role of integrating theoretical and experimental approaches, beyond just high-harmonic spectroscopy, for the development of versatile harmonic spectroscopic probes of charge migration.

中文翻译：

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多维分子高次谐波光谱：电荷迁移研究路线图

摘要 本综述讨论了小分子高次谐波光谱的最新实验和理论分析，目的是表征电荷迁移。我们讨论了分子高次谐波光谱的制定，以及在实验和从头算模拟中提取分子目标特定信息的方法。我们提供了测量和模拟的二氧化碳和硫化羰的高谐波光谱，以说明对包括光谱幅度和相位的高谐波光谱进行多维分析的必要性。利用这些结果，我们研究了这种多维分析如何为使用高谐波光谱研究电荷迁移铺平道路，并说明静态分子特征在探测动力学时可以发挥的有益作用。最后，