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Issue 19, 2019
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Ultrafast imaging of laser-controlled non-adiabatic dynamics in NO2 from time-resolved photoelectron emission

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Abstract

Time-resolving and controlling coupled electronic and nuclear dynamics at conical intersections on the sub-femtosecond to few-femtosecond time scale is among the challenging goals of attosecond physics. Here we present numerical simulations of time-resolved photoelectron spectroscopy of such dynamics in NO2, where the coupled electron–nuclear motion at the 2A1/2B2 conical intersection is steered on the sub-laser-cycle time scale by a nearly single-cycle, waveform controlled mid-infrared laser pulse. For a rigorous description of the photoionization dynamics, we employ ab initio energy- and geometry-resolved photoionization matrix elements obtained with the multichannel R-matrix method, using a multiconfigurational description of the molecule and a newly developed algorithm to generate photoionization dipoles that are phase consistent on the level of both the neutral and the ionic states. We find that for sufficient molecular alignment, the time- and energy-resolved anisotropy parameters of the photoelectron angular distributions provide a particularly clear picture of both the ultrafast natural molecular dynamics at the conical intersection and its modifications by the control pulse. In particular, changes in the electronic and nuclear configurations induced by the control pulse lead to the appearance of non-vanishing odd anisotropy parameters in the photoelectron spectra. These are absent in the spectra obtained without the control pulse and therefore provide sensitive, background-free diagnostic of the control.

Graphical abstract: Ultrafast imaging of laser-controlled non-adiabatic dynamics in NO2 from time-resolved photoelectron emission

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Article information


Submitted
01 Feb 2019
Accepted
07 Apr 2019
First published
08 Apr 2019

Phys. Chem. Chem. Phys., 2019,21, 10038-10051
Article type
Paper

Ultrafast imaging of laser-controlled non-adiabatic dynamics in NO2 from time-resolved photoelectron emission

M. Richter, J. González-Vázquez, Z. Mašín, D. S. Brambila, A. G. Harvey, F. Morales and F. Martín, Phys. Chem. Chem. Phys., 2019, 21, 10038
DOI: 10.1039/C9CP00649D

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