Time-resolved high-harmonic spectroscopy of nonadiabatic dynamics in NO2

Conical intersection dynamics in NO2 probed by homodyne high-harmonic spectroscopy.

Conical intersections play a crucial role in the chemistry of most polyatomic molecules, ranging from the simplest bimolecular reactions to the photostability of DNA. The real-time study of the associated electronic dynamics poses a major challenge to the latest techniques of ultrafast measurement. We show that high-harmonic spectroscopy reveals oscillations in the electronic character that occ...

Time-resolved photoelectron spectroscopy of wavepackets through a conical intersection in NO2.

We report the results of theoretical studies of the time-resolved femtosecond photoelectron spectroscopy of quantum wavepackets through the conical intersection between the first two (2)A' states of NO(2). The Hamiltonian explicitly includes the pump-pulse interaction, the nonadiabatic coupling due to the conical intersection between the neutral states, and the probe interaction between the neu...

Interrogation of Nonadiabatic Molecular Dynamics via Time-Resolved Photoelectron Spectroscopy

High-harmonic spectroscopy of laser-driven nonadiabatic electron dynamics in the hydrogen molecular ion

We theoretically explore a mechanism resulting in a minimum in the high-harmonic spectrum of a hydrogen molecular ion driven at extended internuclear distances by a mid-infrared laser source. Our analysis identifies this minimum to be a signature of the transient localization of the electron upon alternating nuclear centers and is representative of dynamics occurring exclusively at the time of ...

Femtosecond time - resolved spectroscopy in polyatomic systems investigated by velocity -

Femtosecond time-resolved spectroscopy in polyatomic systems investigated by velocity-map imaging and high-order harmonic generation presented by David STÄDTER Revealing the underlying ultrafast dynamics in molecular reaction spectroscopy demands state-of-the-art imaging techniques to follow a molecular process step by step. Femtosecond time-resolved velocity-map imaging is used to study the ph...