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

Phys Rev Lett. 2007 Oct 19;99(16):163001. doi: 10.1103/PhysRevLett.99.163001. Epub 2007 Oct 16.

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 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.