Coherent ultrafast core-hole correlation spectroscopy: x-ray analogues of multidimensional NMR

TL;DR

This paper introduces a new two-dimensional x-ray spectroscopy technique to study interactions between core-electron and valence transitions, revealing complex many-body effects in molecules.

Contribution

It proposes a novel 2DXCS method for probing core-electron and valence interactions, with potential future experimental applications using high-intensity x-ray sources.

Findings

Spectra show off-diagonal cross-peaks indicating coupling of different core transitions.

Calculations on aminophenol isomers demonstrate extraction of many-body electronic effects.

Method provides new insights into electronic structure and excitations.

Abstract

We propose two dimensional x-ray coherent correlation spectroscopy (2DXCS) for the study of interactions between core-electron and valence transitions. This technique might find experimental applications in the future when very high intensity x-ray sources become available. Spectra obtained by varying two delay periods between pulses show off-diagonal cross-peaks induced by coupling of core transitions of two different types. Calculations of the N1s and O1s signals of aminophenol isomers illustrate how novel information about many-body effects in electronic structure and excitations of molecules can be extracted from these spectra.