Coherent and Incoherent Excitation Pathways in Time-Resolved Photoemission Orbital Tomography of CuPc/Cu(001)-2O

Adamkiewicz, Alexa and Raths, Miriam and Stettner, Monja and Theilen, Marcel and Munster, Lasse and Wenzel, Sabine and Hutter, Mark and Soubatch, Serguei and Kumpf, Christian and Bocquet, Francois C. and Wallauer, Robert and Tautz, F. Stefan and Hofer, Ulrich (2023) Coherent and Incoherent Excitation Pathways in Time-Resolved Photoemission Orbital Tomography of CuPc/Cu(001)-2O. JOURNAL OF PHYSICAL CHEMISTRY C, 127 (41). pp. 20411-20418. ISSN 1932-7447, 1932-7455

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Abstract

Time-resolved photoemission orbital tomography (tr-POT) offers unique possibilities for tracing molecular electron dynamics. The recorded pump-induced changes of the angle-resolved photoemission intensities allow one to characterize unoccupied molecular states in momentum space and to deduce the incoherent temporal evolution of their population. Here, we show for the example of CuPc/Cu(001)-2O that the method also gives access to the coherent regime and that different excitation pathways can be disentangled by a careful analysis of the time-dependent change of the photoemission momentum pattern. In particular, we demonstrate by varying photon energy and polarization of the pump light how the incoherent temporal evolution of the LUMO distribution can be distinguished from coherent contributions of the projected HOMO. Moreover, we report the selective excitation of molecules with a specific orientation at normal incidence by aligning the electric field of the pump light along the molecular axis.

Item Type: Article
Uncontrolled Keywords: ELECTRONIC-STRUCTURE; DYNAMICS;
Subjects: 500 Science > 530 Physics
Divisions: Physics > Institute of Experimental and Applied Physics
Depositing User: Dr. Gernot Deinzer
Date Deposited: 16 Mar 2024 12:24
Last Modified: 16 Mar 2024 12:24
URI: https://pred.uni-regensburg.de/id/eprint/60174

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