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Phys Chem Chem Phys. 2011 Nov 7;13(41):18447-67. doi: 10.1039/c1cp22031d. Epub 2011 Sep 22.

Time-resolved photoelectron spectroscopy: from wavepackets to observables.

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Steacie Institute for Molecular Sciences, National Research Council, 100 Sussex Drive, Ottawa, Ontario K1A 0R6, Canada.


Time-resolved photoelectron spectroscopy (TRPES) is a powerful tool for the study of intramolecular dynamics, particularly excited state non-adiabatic dynamics in polyatomic molecules. Depending on the problem at hand, different levels of TRPES measurements can be performed: time-resolved photoelectron yield; time- and energy-resolved photoelectron yield; time-, energy-, and angle-resolved photoelectron yield. In this pedagogical overview, a conceptual framework for time-resolved photoionization measurements is presented, together with discussion of relevant theory for the different aspects of TRPES. Simple models are used to illustrate the theory, and key concepts are further amplified by experimental examples. These examples are chosen to show the application of TRPES to the investigation of a range of problems in the excited state dynamics of molecules: from the simplest vibrational wavepacket on a single potential energy surface; to disentangling intrinsically coupled electronic and nuclear motions; to identifying the electronic character of the intermediate states involved in non-adiabatic dynamics by angle-resolved measurements in the molecular frame, the most complete measurement.


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