Multidimensional electronic spectroscopy in high-definition-Combining spectral, temporal, and spatial resolutions.
Multidimensional electronic spectroscopy in high-definition-Combining spectral, temporal, and spatial resolutions.
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高清多维电子光谱——结合光谱、时间和空间分辨率。
DOI：
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发表时间：
2021
影响因子：
4.4
通讯作者：
V. Tiwari
中科院分区：
文献类型：
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作者：
V. Tiwari
在过去的二十年里，相干多维光谱已经在电磁频谱的太赫兹，红外，可见光和紫外区域实现。几个共振的相干激发与几个周期的脉冲相结合，以及沿着沿着多个光谱维度的光谱去拥挤，使人们对广泛的分子尺度现象有了新的认识，例如自然和人工光捕获系统中的能量和电荷离域，单层中的氢键动力学，以及法布里-珀罗腔中的强光-物质耦合。然而，对合奏的测量已经暗示了相关细节上的信号平均，例如形态和能量不均匀性，这些不均匀性不被傅立叶变换重新定相。最近扩展这些光谱，以提供衍射有限的空间分辨率，同时保持时间和光谱信息，一直令人兴奋，并铺平了道路，以解决几个具有挑战性的问题，超越合奏平均。本透视图的目的是讨论最终实现空间分辨多维电子光谱的技术发展，并强调通过在强大的光谱工具中引入空间分辨率而实现的一些最新发现。
Over the past two decades, coherent multidimensional spectroscopies have been implemented across the terahertz, infrared, visible, and ultraviolet regions of the electromagnetic spectrum. A combination of coherent excitation of several resonances with few-cycle pulses, and spectral decongestion along multiple spectral dimensions, has enabled new insights into wide ranging molecular scale phenomena, such as energy and charge delocalization in natural and artificial light-harvesting systems, hydrogen bonding dynamics in monolayers, and strong light-matter couplings in Fabry-Pérot cavities. However, measurements on ensembles have implied signal averaging over relevant details, such as morphological and energetic inhomogeneity, which are not rephased by the Fourier transform. Recent extension of these spectroscopies to provide diffraction-limited spatial resolution, while maintaining temporal and spectral information, has been exciting and has paved a way to address several challenging questions by going beyond ensemble averaging. The aim of this Perspective is to discuss the technological developments that have eventually enabled spatially resolved multidimensional electronic spectroscopies and highlight some of the very recent findings already made possible by introducing spatial resolution in a powerful spectroscopic tool.