Tiwari, V (2021) Multidimensional electronic spectroscopy in high-definition—Combining spectral, temporal, and spatial resolutions. In: Journal of Chemical Physics, 154 (23). 1ENG.
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Abstract
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. © 2021 Author(s).
| Item Type: | Journal Article |
|---|---|
| Publication: | Journal of Chemical Physics |
| Publisher: | American Institute of Physics Inc. |
| Additional Information: | The copyright for this article belongs to Authors. |
| Keywords: | Hydrogen bonds; Image resolution, Artificial light harvesting; Charge delocalization; Diffraction limited spatial resolution; Electromagnetic spectra; Electronic spectroscopy; Hydrogen bonding dynamics; Multidimensional spectroscopy; Technological development, Terahertz spectroscopy |
| Department/Centre: | Division of Chemical Sciences > Solid State & Structural Chemistry Unit |
| Date Deposited: | 31 Aug 2021 06:36 |
| Last Modified: | 16 May 2023 09:28 |
| URI: | https://eprints.iisc.ac.in/id/eprint/69479 |
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