阿秒
高次谐波产生
谐波
电离
光谱学
原子物理学
激光器
物理
电子
调制(音乐)
信号(编程语言)
谐波
光学
超短脉冲
离子
计算机科学
电压
量子力学
声学
程序设计语言
作者
Kyle A. Hamer,Aderonke S. Folorunso,Kenneth A. Lopata,Kenneth J. Schafer,Mette B. Gaarde,F. Mauger
标识
DOI:10.1021/acs.jpca.3c04234
摘要
We present frequency-matched strobo-spectroscopy (FMSS) of charge migration (CM) in bromobutadiyne, simulated with time-dependent density functional theory. CM + FMSS is a pump–probe scheme that uses a frequency-matched high harmonic generation (HHG)-driving laser as an independent probe step, following the creation of a localized hole on the bromine atom that induces CM dynamics. We show that the delay-dependent harmonic yield tracks the phase of the CM dynamics through its sensitivity to the amount of electron density on the bromine end of the molecule. FMSS takes advantage of the intrinsic attosecond time resolution of the HHG process in which different harmonics are emitted at different times and thus probe different locations of the electron hole. Finally, we show that the CM-induced modulation of the HHG signal is dominated by the recombination step of the HHG process, with a negligible contribution from the ionization step.
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