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 (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.

References in corpus (2)

• Tracing ultrafast interatomic electronic decay processes in real time and space
• Double-quantum-coherence attosecond x-ray spectroscopy of spatially separated, spectrally overlapping core-electron transitions

Cited by in corpus (6)

• Molecular chirality and its monitoring by ultrafast X-ray pulses
• Manipulating Core-Excitations in Molecules by X-ray Cavities
• Transient Impulsive Giant Electronic Raman Redistribution
• Stochastic Liouville Equations for Femtosecond Stimulated Raman Spectroscopy
• Coupled cluster simulation of impulsive stimulated X-ray Raman scattering
• Effects of Structural Variations to X-ray Absorption Spectra of g-C${}_3$N${}_4$: Insights from DFT and TDDFT Simulations