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Issue 23, 2021
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Manipulating valence and core electronic excitations of a transition-metal complex using UV/Vis and X-ray cavities

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Abstract

We demonstrate how optical cavities can be exploited to control both valence- and core-excitations in a prototypical model transition metal complex, ferricyanide ([Fe(III)(CN)6]3−), in an aqueous environment. The spectroscopic signatures of hybrid light-matter polariton states are revealed in UV/Vis and X-ray absorption, and stimulated X-ray Raman signals. In an UV/Vis cavity, the absorption spectrum exhibits the single-polariton states arising from the cavity photon mode coupling to both resonant and off-resonant valence-excited states. We further show that nonlinear stimulated X-ray Raman signals can selectively probe the bipolariton states via cavity-modified Fe core-excited states. This unveils the correlation between valence polaritons and dressed core-excitations. In an X-ray cavity, core-polaritons are generated and their correlations with the bare valence-excitations appear in the linear and nonlinear X-ray spectra.

Graphical abstract: Manipulating valence and core electronic excitations of a transition-metal complex using UV/Vis and X-ray cavities

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Supplementary files

Article information


Submitted
29 Mar 2021
Accepted
02 May 2021
First published
06 May 2021

This article is Open Access
All publication charges for this article have been paid for by the Royal Society of Chemistry

Chem. Sci., 2021,12, 8088-8095
Article type
Edge Article

Manipulating valence and core electronic excitations of a transition-metal complex using UV/Vis and X-ray cavities

B. Gu, S. M. Cavaletto, D. R. Nascimento, M. Khalil, N. Govind and S. Mukamel, Chem. Sci., 2021, 12, 8088
DOI: 10.1039/D1SC01774H

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