Coherent Ultrafast Core-Hole Correlation Spectroscopy: X-Ray Analogues of Multidimensional NMR

Abstract

We propose two-dimensional x-ray coherent correlation spectroscopy for the study of interactions between core-electron and valence transitions. This technique may 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 crosspeaks induced by coupling of core transitions of two different types. Calculations of the $\mathrm{N}1s$ and $\mathrm{O}1s$ 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.