Capturing Fingerprints of Conical Intersection: Complementary Information of Non-Adiabatic Dynamics from Linear X-ray Probes

Abstract

Many recent experimental ultrafast spectroscopy studies have hinted at non-adiabatic dynamics indicating the existence of conical intersections, but their direct observation remains a challenge. The rapid change of the energy gap between the electronic states complicated their observation by requiring bandwidths of several electron volts. In this manuscript, we propose to use the combined information of different X-ray pump-probe techniques to identify the conical intersection. We theoretically study the conical intersection in pyrrole using transient X-ray absorption, time-resolved X-ray spontaneous emission, and linear off-resonant Raman spectroscopy to gather evidence of the curve crossing.

References in corpus (8)

• Nonlinear optical signals and spectroscopy with quantum light
• Catching Conical Intersections in the Act; Monitoring Transient Electronic Coherences by Attosecond Stimulated X-Ray Raman Signals
• Ultrafast X-ray spectroscopy of conical intersections
• Nonlinear optical spectroscopy of single, few, and many molecules; nonequilibrium Green's function QED approach
• Visualizing Conical Intersection Passages via Vibronic Coherence Maps Generated by Stimulated Ultrafast X--Ray Raman Signals
• Transient Resonant Auger-Meitner Spectra of Photoexcited Thymine
• Detecting Electronic Coherence by Multidimensional Broadband Stimulated X-Ray Raman Signals
• Detecting coherent core-hole wave-packet dynamics in N2 by time- and angle-resolved inner-shell photoelectron spectroscopy