The stimulated x-ray Raman signal has been calculated for the amino acid cysteine using broadband (FWHM ?14.2eV, 128 as) pulses tuned to the nitrogen K-edge. Peaks correspond to those valence excited states and reveal electronic Frank-Condon overlaps between canonical valence orbitals and relaxed orbitals in the presence of the core hole. The coupling between excited states with valence- and core-holes is further explored using a coherent, wave-vector matched photon echo technique, where it is possible to eliminate stimulated emission and excited-state absorption by taking the waiting time to be longer the lifetime of the core hole (~ 7:1 fs for nitrogen).
Revised: December 13, 2013 |
Published: March 13, 2013
Citation
Biggs J.D., Y. Zhang, D. Healion, N. Govind, and S. Mukamel. 2013.Dissecting X-Ray Raman Resonances Using Four-Wave Mixing. In Proceedings of the XVIIIth International Conference on Ultrafast Phenomena, July 8-13, 2012, Lausanne, Switzerland, 41, 05040-1 to 05040-3. Les Ulis:EDP Sciences.PNNL-SA-89220.doi:10.1051/epjconf/20134105040