Journal Article

PUBDB-2022-00404

http://join2-wiki.gsi.de/foswiki/pub/Main/Artwork/join2_logo100x88.png Ultrafast Adsorbate Excitation Probed with Subpicosecond-Resolution X-Ray Absorption Spectroscopy

Diesen, E. (Corresponding author) ; Wang, H.-Y. ; Schreck, S. ; Weston, M. ; Ogasawara, H. ; LaRue, J. ; Perakis, F. ; Dell’Angela, M. ; Capotondi, F. ; Giannessi, L. ; Pedersoli, E. ; Naumenko, D. ; Nikolov, I. ; Raimondi, L. ; Spezzani, C. ; Beye, M.XFEL.EU*DESY* ; Cavalca, F. ; Liu, B. ; Gladh, J. ; Koroidov, S. ; Miedema, P.XFEL.EU*DESY* ; Costantini, R. ; Heinz, T. F. ; Abild-Pedersen, F. ; Voss, J. ; Luntz, A. C. ; Nilsson, A.

2021
APS College Park, Md.

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Please use a persistent id in citations: doi:10.1103/PhysRevLett.127.016802  doi:10.3204/PUBDB-2022-00404

Abstract: We use a pump-probe scheme to measure the time evolution of the C K-edge x-ray absorption spectrum from CO/Ru(0001) after excitation by an ultrashort high-intensity optical laser pulse. Because of the short duration of the x-ray probe pulse and precise control of the pulse delay, the excitation-induced dynamics during the first picosecond after the pump can be resolved with unprecedented time resolution. By comparing with density functional theory spectrum calculations, we find high excitation of the internal stretch and frustrated rotation modes occurring within 200 fs of laser excitation, as well as thermalization of the system in the picosecond regime. The ∼100  fs initial excitation of these CO vibrational modes is not readily rationalized by traditional theories of nonadiabatic coupling of adsorbates to metal surfaces, e.g., electronic frictions based on first order electron-phonon coupling or transient population of adsorbate resonances. We suggest that coupling of the adsorbate to nonthermalized electron-hole pairs is responsible for the ultrafast initial excitation of the modes.

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Contributing Institute(s):

1. FS-FLASH (CFEL-UDSS)

Research Program(s):

1. 631 - Matter – Dynamics, Mechanisms and Control (POF4-631) (POF4-631)

Experiment(s):

1. Measurement at external facility

Appears in the scientific report 2021

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Database coverage:
; ; ; Clarivate Analytics Master Journal List ; Current Contents - Electronics and Telecommunications Collection ; Current Contents - Physical, Chemical and Earth Sciences ; Ebsco Academic Search ; Essential Science Indicators ; IF >= 5 ; JCR ; Nationallizenz ; SCOAP3 sponsored Journal ; SCOPUS ; Science Citation Index Expanded ; Web of Science Core Collection

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