Journal Article

FZJ-2021-01342

http://join2-wiki.gsi.de/foswiki/pub/Main/Artwork/join2_logo100x88.png Tracing orbital images on ultrafast time scales

Wallauer, R. ; Raths, M.FZJ* ; Stallberg, K. ; Münster, L. ; Brandstetter, D. ; Yang, X.FZJ* ; Güdde, J. ; Puschnig, P. ; Soubatch, S.FZJ* ; Kumpf, C.FZJ* ; Bocquet, F. C.FZJ* ; Tautz, F. S. (Corresponding author)FZJ* ; Höfer, U. (Corresponding author)

2021
Assoc.73085 Washington, DC

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Please use a persistent id in citations: http://hdl.handle.net/2128/27902  doi:10.1126/science.abf3286

Abstract: Frontier orbitals determine fundamental molecular properties such as chemical reactivities. Although electron distributions of occupied orbitals can be imaged in momentum space by photoemission tomography, it has so far been impossible to follow the momentum-space dynamics of a molecular orbital in time, for example, through an excitation or a chemical reaction. Here, we combined time-resolved photoemission using high laser harmonics and a momentum microscope to establish a tomographic, femtosecond pump-probe experiment of unoccupied molecular orbitals. We measured the full momentum-space distribution of transiently excited electrons, connecting their excited-state dynamics to real-space excitation pathways. Because in molecules this distribution is closely linked to orbital shapes, our experiment may, in the future, offer the possibility of observing ultrafast electron motion in time and space.

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Contributing Institute(s):

1. Funktionale Nanostrukturen an Oberflächen (PGI-3)

Research Program(s):

1. 521 - Quantum Materials (POF4-521) (POF4-521)
2. DFG project 396769409 - Grundlagen der Photoemissionstomographie (396769409)

Appears in the scientific report 2021

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