title: Two-dimensional stimulated resonance Raman spectroscopy of molecules with broadband x-ray pulses.
abstract: 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 (181 as, 14.2 eV FWHM) 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.
authors.affiliation: Department of Chemistry, University of California, Irvine, California 92697-2025, USA.
authors.forename: Jason D
authors.initials: JD
authors.lastname: Biggs
authors.forename: Yu
authors.initials: Y
authors.lastname: Zhang
authors.forename: Daniel
authors.initials: D
authors.lastname: Healion
authors.forename: Shaul
authors.initials: S
authors.lastname: Mukamel
mesh_terms: D003198:Computer Simulation; D004583:Electrons; D009584:Nitrogen / Q000737:chemistry*; D010100:Oxygen / Q000737:chemistry*; D013059:Spectrum Analysis, Raman; D014732:Vibration; D014965:X-Rays
chemical_list: D009584:Nitrogen; D010100:Oxygen