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Phys. Rev. Lett. 99, 163001 (2007) [4 pages]Coherent Ultrafast Core-Hole Correlation Spectroscopy: X-Ray Analogues of Multidimensional NMR
Received 22 December 2006; published 16 October 2007
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. ©2007 The American Physical Society
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