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Ultrafast molecular frame electronic coherences from lab frame scattering anisotropies

From National Research Council Canada

DOIResolve DOI: https://doi.org/10.1088/1361-6455/ab7a84
AuthorSearch for: ORCID identifier: https://orcid.org/0000-0002-4975-4888; Search for: ORCID identifier: https://orcid.org/0000-0001-5917-4417; Search for: 1; Search for: ; Search for: 1; Search for: 1; Search for: ; Search for: ; Search for: 1; Search for: 1ORCID identifier: https://orcid.org/0000-0002-8447-3678
Affiliation
  1. National Research Council of Canada. Security and Disruptive Technologies
FormatText, Article
Subjectelectronic coherence; non-adiabatic molecular dynamics; molecular photoionization; photoelectron angular distributions; ultrafast molecular dynamics; molecular alignment; molecular frame measurement
Abstract
Electronic coherences in molecules are ultrafast charge oscillations on the molecular frame (MF) and their direct observation and separation from electronic population dynamics is challenging. Here we present a valence shell lab frame (LF) scattering method suited to probing electronic coherences in isolated systems. MF electronic coherences lead to LF electronic anisotropies observable by ultrafast angle-resolved scattering. Moment analysis of the LF anisotropy completely separates electronic coherences from population dynamics, demonstrated in excited state NH3 using ultrafast time-energy-angle-resolved photoelectron spectroscopy. This general approach applies equally to attosecond/femtosecond electronic coherences in isolated systems.
Publication date
PublisherIOP Publishing
In
  • Journal of Physics B: Atomic, Molecular and Optical Physics 53, no. 11, 114001 (5 May 2020): 1–12.
LanguageEnglish
Peer reviewedYes
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Record identifier1b09e825-bd65-4e6e-9188-8c687301e917
Record created2020-06-29
Record modified2023-08-11
Date modified: