Conical-intersection dynamics and ground-state chemistry probed by extreme-ultraviolet time-resolved photoelectron spectroscopy

A. von Conta, A. Tehlar, A. Schletter, Y. Arasaki, K. Takatsuka and H. J. Wörner ()
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A. von Conta: ETH Zurich
A. Tehlar: ETH Zurich
A. Schletter: ETH Zurich
Y. Arasaki: Kyoto University
K. Takatsuka: Kyoto University
H. J. Wörner: ETH Zurich

Nature Communications, 2018, vol. 9, issue 1, 1-10

Abstract: Abstract Time-resolved photoelectron spectroscopy (TRPES) is a useful approach to elucidate the coupled electronic-nuclear quantum dynamics underlying chemical processes, but has remained limited by the use of low photon energies. Here, we demonstrate the general advantages of XUV-TRPES through an application to NO2, one of the simplest species displaying the complexity of a non-adiabatic photochemical process. The high photon energy enables ionization from the entire geometrical configuration space, giving access to the true dynamics of the system. Specifically, the technique reveals dynamics through a conical intersection, large-amplitude motion and photodissociation in the electronic ground state. XUV-TRPES simultaneously projects the excited-state wave packet onto many final states, offering a multi-dimensional view of the coupled electronic and nuclear dynamics. Our interpretations are supported by ab initio wavepacket calculations on new global potential-energy surfaces. The presented results contribute to establish XUV-TRPES as a powerful technique providing a complete picture of ultrafast chemical dynamics from photoexcitation to the final products.

Date: 2018
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DOI: 10.1038/s41467-018-05292-4

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