4.6 Article

Improved insights in time-resolved photoelectron imaging

Journal

PHYSICAL CHEMISTRY CHEMICAL PHYSICS
Volume 23, Issue 18, Pages 10736-10755

Publisher

ROYAL SOC CHEMISTRY
DOI: 10.1039/d1cp00933h

Keywords

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Funding

  1. Engineering and Physical Sciences Research Council [EP/G041717/1, EP/K021052/1, EP/P001459/1, EP/R030448/1]
  2. Heriot-Watt University
  3. EPSRC [EP/K021052/1, EP/P001459/1, EP/G041717/1, EP/R030448/1] Funding Source: UKRI

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Time-resolved photoelectron imaging (TRPEI) is a highly differential technique used to study the dynamics of non-adiabatic energy redistribution in electronically excited states of molecules. While the method has broad research significance, there are limitations that need to be addressed. Through various examples, challenges commonly encountered in the analysis and interpretation of experimental data are illustrated, along with initial thoughts on potential solutions.
Time-resolved photoelectron imaging (TRPEI) is a highly differential technique for the detailed study of non-adiabatic energy redistribution dynamics operating in the electronically excited states of molecules following the absorption of ultraviolet light. This Perspective briefly reviews the main elements of the TRPEI method but also seeks to address some of its limitations. With the help of various examples drawn from our own recent work, we illustrate some of the challenges commonly encountered during the analysis and interpretation of experimental data and introduce some initial thoughts on approaches to help deal with them. We also discuss some novel methods that aim to expand the capabilities and utility of the TRPEI technique by extending the observation window along the photochemical reaction coordinate(s) and improving the temporal resolution. Given the widespread use of TRPEI and related ultrafast spectroscopies, we anticipate that this Perspective will be of broad interest to a sizeable research community. Furthermore, we hope it will also serve as a useful overview for those engaging with this topic for the first time.

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