Manipulating Core Excitations in Molecules by X-Ray Cavities

Bing Gu, Artur Nenov, Francesco Segatta, Marco Garavelli, and Shaul Mukamel

Phys. Rev. Lett. 126, 053201 – Published 4 February 2021

Abstract

Core excitations on different atoms are highly localized and therefore decoupled. By placing molecules in an x-ray cavity the core transitions become coupled via the exchange of cavity photons and form delocalized hybrid light-matter excitations known as core polaritons. We demonstrate these effects for the two inequivalent carbon atoms in 1,1-difluoroethylene. Polariton signatures in the x-ray absorption, two-photon absorption, and multidimensional four-wave mixing signals are predicted.

Received 27 August 2020
Revised 2 December 2020
Accepted 22 December 2020

DOI:https://doi.org/10.1103/PhysRevLett.126.053201

Physics Subject Headings (PhySH)

Electronic excitation & ionization Strong electromagnetic field effects

Molecules

X-ray absorption near-edge spectroscopy

Atomic, Molecular & OpticalGeneral Physics

Authors & Affiliations

Bing Gu ^1,*, Artur Nenov^2,*, Francesco Segatta², Marco Garavelli^2,†, and Shaul Mukamel ^1,‡

¹Department of Chemistry and Department of Physics and Astronomy, University of California, Irvine, California 92697, USA
²Dipartimento di Chimica Industriale “Toso Montanari,” Università degli studi di Bologna, Viale del Risorgimento 4, 40136 Bologna, Italy