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000891059 1001_ $$0P:(DE-HGF)0$$aWallauer, R.$$b0
000891059 245__ $$aTracing orbital images on ultrafast time scales
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000891059 520__ $$aFrontier orbitals determine fundamental molecular properties such as chemical reactivities. Although electron distributions of occupied orbitals can be imaged in momentum space by photoemission tomography, it has so far been impossible to follow the momentum-space dynamics of a molecular orbital in time, for example, through an excitation or a chemical reaction. Here, we combined time-resolved photoemission using high laser harmonics and a momentum microscope to establish a tomographic, femtosecond pump-probe experiment of unoccupied molecular orbitals. We measured the full momentum-space distribution of transiently excited electrons, connecting their excited-state dynamics to real-space excitation pathways. Because in molecules this distribution is closely linked to orbital shapes, our experiment may, in the future, offer the possibility of observing ultrafast electron motion in time and space.
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000891059 7001_ $$0P:(DE-Juel1)172607$$aRaths, M.$$b1
000891059 7001_ $$0P:(DE-HGF)0$$aStallberg, K.$$b2
000891059 7001_ $$0P:(DE-HGF)0$$aMünster, L.$$b3
000891059 7001_ $$0P:(DE-HGF)0$$aBrandstetter, D.$$b4
000891059 7001_ $$0P:(DE-Juel1)165181$$aYang, X.$$b5
000891059 7001_ $$0P:(DE-HGF)0$$aGüdde, J.$$b6
000891059 7001_ $$0P:(DE-HGF)0$$aPuschnig, P.$$b7
000891059 7001_ $$0P:(DE-Juel1)128790$$aSoubatch, S.$$b8
000891059 7001_ $$0P:(DE-Juel1)128774$$aKumpf, C.$$b9
000891059 7001_ $$0P:(DE-Juel1)167128$$aBocquet, F. C.$$b10
000891059 7001_ $$0P:(DE-Juel1)128791$$aTautz, F. S.$$b11$$eCorresponding author
000891059 7001_ $$0P:(DE-HGF)0$$aHöfer, U.$$b12$$eCorresponding author
000891059 773__ $$0PERI:(DE-600)2089761-3$$a10.1126/science.abf3286$$gVol. 371, no. 6533, p. 1056 - 1059$$n6533$$p1056 - 1059$$tScience / Science now$$v371$$x1095-9203$$y2021
000891059 8564_ $$uhttps://juser.fz-juelich.de/record/891059/files/1056.full-1.pdf
000891059 8564_ $$uhttps://juser.fz-juelich.de/record/891059/files/67855.pdf
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