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.
journal_name
Nat Communjournal_title
Nature communicationsauthors
von Conta A,Tehlar A,Schletter A,Arasaki Y,Takatsuka K,Wörner HJdoi
10.1038/s41467-018-05292-4subject
Has Abstractpub_date
2018-08-08 00:00:00pages
3162issue
1issn
2041-1723pii
10.1038/s41467-018-05292-4journal_volume
9pub_type
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