Hannover 2013 – wissenschaftliches Programm
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MO: Fachverband Molekülphysik
MO 15: Femtosecond Spectroscopy IV
MO 15.4: Vortrag
Mittwoch, 20. März 2013, 12:00–12:15, F 102
Ultrafast X-ray photoelectron spectroscopy studies of photoinduced electronic dynamics in dye sensitized semiconductor nanocrystals. — •Katrin Siefermann1,2, Fabian Weise1, Ming-Fu Lin1, Camila Bacellar1, Ali Belkacem1, Thorsten Weber1, Felix Sturm1, Daniel Slaughter1, Champak Khurmi1, Travis Wright1, Bob Schoenlein1, Matthew Strader1, Hana Cho1, Robert Kaindl1, Giacomo Coslovich1, David Prendergast1, Andrey Shavorskiy1, Hendrik Bluhm1, Jinghua Guo1, Marcus Hertlein1, Tolek Tyliszczak1, Amy Cordones3, Josh Vura-Weis3, Stephen Leone3, Daniel Neumark3, Sheraz Gul4, Jin Zhang4, Nils Huse5, Martin Beye6, Anders Nilsson7, Hirohito Ogasawara7, Dennis Nordlund7, Josh Turner7, Bill Schlotter7, Oleg Krupin7, Michael Holmes7, Mike Minitti7, Joseph Robinson7, Marc Messerschmidt7, Phil Heimann7, and Oliver Gessner1 — 1Lawrence Berkeley National Laboratory, Berkeley, USA — 2Leibniz Institute of Surface Modification, Leipzig, Germany — 3University of California Berkeley, USA — 4University of California Santa Cruz, USA — 5Center for Free Electron Laser Science, Hamburg, Germany — 6Helmholtz Zentrum Berlin, Germany — 7SLAC National Accelerator Laboratory, Stanford, USA
We present time-resolved X-ray photoelectron spectroscopy (TRXPS) as a tool to investigate ultrafast dynamics in complex systems in real time. In a proof-of-principle experiment at the Linac Coherent Light Source (LCLS) at SLAC, we monitored the photoinduced oxidation state change of a Ruthenium-based dye complex (N3) attached to zinc oxide nanocrystals. This system is a critical component of dye-sensitized solar cells. In our experiment, an ultrashort laser pulse with a center wavelength of 535 nm electronically excites the Ru dye complex. A time-delayed X-ray pulse centered at ∼850 eV is used to record the inner shell photoelectron spectrum of the sample in the region of the Ru 3d3/2,5/2 lines. Oxidation of the dye is detected at a pump-probe delay of ∼500 fs as a transient shift of the Ru 3d photoelectron lines by ∼2 eV toward higher binding energies. The experiment represents a first step toward an atomic site specific real-time picture of charge migration in dye sensitized solar cells and demonstrates the potential of time-resolved X-ray photoelectron spectroscopy (TRXPS) as a tool to investigate ultrafast electronic dynamics in complex systems.