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000473986 1001_ $$00000-0002-8235-3920$$aDiesen, Elias$$b0$$eCorresponding author
000473986 245__ $$aUltrafast Adsorbate Excitation Probed with Subpicosecond-Resolution X-Ray Absorption Spectroscopy
000473986 260__ $$aCollege Park, Md.$$bAPS$$c2021
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000473986 520__ $$aWe use a pump-probe scheme to measure the time evolution of the C K-edge x-ray absorption spectrum from CO/Ru(0001) after excitation by an ultrashort high-intensity optical laser pulse. Because of the short duration of the x-ray probe pulse and precise control of the pulse delay, the excitation-induced dynamics during the first picosecond after the pump can be resolved with unprecedented time resolution. By comparing with density functional theory spectrum calculations, we find high excitation of the internal stretch and frustrated rotation modes occurring within 200 fs of laser excitation, as well as thermalization of the system in the picosecond regime. The ∼100  fs initial excitation of these CO vibrational modes is not readily rationalized by traditional theories of nonadiabatic coupling of adsorbates to metal surfaces, e.g., electronic frictions based on first order electron-phonon coupling or transient population of adsorbate resonances. We suggest that coupling of the adsorbate to nonthermalized electron-hole pairs is responsible for the ultrafast initial excitation of the modes.
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000473986 7001_ $$aWang, Hsin-Yi$$b1
000473986 7001_ $$aSchreck, Simon$$b2
000473986 7001_ $$aWeston, Matthew$$b3
000473986 7001_ $$aOgasawara, Hirohito$$b4
000473986 7001_ $$aLaRue, Jerry$$b5
000473986 7001_ $$aPerakis, Fivos$$b6
000473986 7001_ $$aDell’Angela, Martina$$b7
000473986 7001_ $$aCapotondi, Flavio$$b8
000473986 7001_ $$aGiannessi, Luca$$b9
000473986 7001_ $$aPedersoli, Emanuele$$b10
000473986 7001_ $$aNaumenko, Denys$$b11
000473986 7001_ $$aNikolov, Ivaylo$$b12
000473986 7001_ $$aRaimondi, Lorenzo$$b13
000473986 7001_ $$aSpezzani, Carlo$$b14
000473986 7001_ $$0P:(DE-H253)PIP1005334$$aBeye, Martin$$b15
000473986 7001_ $$aCavalca, Filippo$$b16
000473986 7001_ $$aLiu, Boyang$$b17
000473986 7001_ $$aGladh, Jörgen$$b18
000473986 7001_ $$aKoroidov, Sergey$$b19
000473986 7001_ $$0P:(DE-H253)PIP1032830$$aMiedema, Piter$$b20
000473986 7001_ $$aCostantini, Roberto$$b21
000473986 7001_ $$aHeinz, Tony F.$$b22
000473986 7001_ $$aAbild-Pedersen, Frank$$b23
000473986 7001_ $$aVoss, Johannes$$b24
000473986 7001_ $$aLuntz, Alan C.$$b25
000473986 7001_ $$aNilsson, Anders$$b26
000473986 773__ $$0PERI:(DE-600)1472655-5$$a10.1103/PhysRevLett.127.016802$$gVol. 127, no. 1, p. 016802$$n1$$p016802$$tPhysical review letters$$v127$$x0031-9007$$y2021
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