1204.5795 (Jason D. Biggs et al.)

Two-Dimensional Stimulated Resonance Raman Spectroscopy of Molecules
with Broadband X-ray Pulses    [PDF]

Jason D. Biggs, Yu Zhang, Daniel Healion, Shaul Mukamel

Expressions for the two-dimensional Stimulated x-ray Raman Spectroscopy (2D-SXRS) signal obtained using attosecond x-ray pulses are derived. The 1D- and 2D-SXRS signals are calculated for trans-N-methyl acetamide (NMA) with broad bandwidth (FWHM ~14.2eV, 181 as) pulses tuned to the oxygen and nitrogen K-edges. Crosspeaks in 2D signals reveal electronic Franck-Condon overlaps between valence orbitals and relaxed orbitals in the presence of the core hole.

View original: http://arxiv.org/abs/1204.5795