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 (7)

• Resonant Inelastic X-ray Scattering Studies of Elementary Excitations
• Coherent methods in the X-ray sciences
• Extreme-ultraviolet pump-probe studies of one femtosecond scale electron dynamics
• Biomolecular imaging and electronic damage using X-ray free-electron lasers
• 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
• Using Wave-Packet Interferometry to Monitor the External Vibrational Control of Electronic Excitation Transfer

Cited by in corpus (13)

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• X-Ray sum frequency generation; direct imaging of ultrafast electron dynamics
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• Manipulating Core-Excitations in Molecules by X-ray Cavities
• Detecting Electronic Coherence by Multidimensional Broadband Stimulated X-Ray Raman Signals
• Double-core Excitations in Formamide Can Be Probed by X-ray Double-quantum-coherence Spectroscopy
• Transient Impulsive Giant Electronic Raman Redistribution
• Stochastic Liouville Equations for Femtosecond Stimulated Raman Spectroscopy
• Nonlinear light scattering in molecules triggered by an impulsive X-ray Raman process
• Optimized pulses for Raman excitation through the continuum: verification using multi-configurational time-dependent Hartree-Fock
• 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