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Multidimensional spectroscopy with attosecond extreme ultraviolet and shaped near-infrared pulses

机译:具有亚秒级极紫外光和成形的近红外脉冲的多维光谱

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摘要

Dynamics following excitation with attosecond extreme ultraviolet (XUV) pulses arise from enormous numbers of accessible excited states, complicating the retrieval of state-specific time evolutions. We develop attosecond XUV multidimensional spectroscopy here to separate interfering pathways on a near-infrared (NIR) energy axis, retrieving single state dynamics in argon atoms in a two-dimensional (2D) XUV-NIR spectrum. In this experiment, we measure four-wave mixing signal arising from the interaction of XUV attosecond pulses centered around 15 eV with two few-cycle NIR pulses. The 2D spectrum is created by measuring the emitted XUV signal field spectrum while applying narrowband amplitude and phase modulations to one of the NIR pulses. Application of such a technique to systems of high dimensionality will provide for the observation of state-resolved pure electronic dynamics, in direct analogy to phenomena unraveled by multidimensional spectroscopies at optical frequencies.
机译:使用亚秒级极紫外(XUV)脉冲激发后的动力学是由大量可访问的激发态引起的,这使状态特定时间演化的检索变得复杂。我们在这里开发了十亿分之一的XUV多维光谱学,以分离近红外(NIR)能量轴上的干扰路径,从而在二维(2D)XUV-NIR光谱中检索氩原子中的单态动态。在本实验中,我们测量了以15 eV为中心的XUV阿秒脉冲与两个短周期NIR脉冲的相互作用所产生的四波混合信号。通过测量发射的XUV信号场谱来创建2D谱,同时将窄带幅度和相位调制应用于NIR脉冲之一。这种技术在高维系统上的应用将提供对状态解析纯电子动力学的观察,这直接类似于多维光谱在光学频率上揭示的现象。

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