Direct observation of charge separation in an organic light harvesting system by femtosecond time-resolved XPS

Friedrich Roth (), Mario Borgwardt, Lukas Wenthaus, Johannes Mahl, Steffen Palutke, Günter Brenner, Giuseppe Mercurio, Serguei Molodtsov, Wilfried Wurth, Oliver Gessner () and Wolfgang Eberhardt ()
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Friedrich Roth: TU Bergakademie Freiberg
Mario Borgwardt: Lawrence Berkeley National Laboratory
Lukas Wenthaus: Center for Free-Electron Laser Science/DESY
Johannes Mahl: Lawrence Berkeley National Laboratory
Steffen Palutke: Deutsches Elektronen-Synchrotron DESY
Günter Brenner: Deutsches Elektronen-Synchrotron DESY
Giuseppe Mercurio: European XFEL GmbH
Serguei Molodtsov: TU Bergakademie Freiberg
Wilfried Wurth: Center for Free-Electron Laser Science/DESY
Oliver Gessner: Lawrence Berkeley National Laboratory
Wolfgang Eberhardt: Center for Free-Electron Laser Science/DESY

Nature Communications, 2021, vol. 12, issue 1, 1-7

Abstract: Abstract The ultrafast dynamics of photon-to-charge conversion in an organic light-harvesting system is studied by femtosecond time-resolved X-ray photoemission spectroscopy (TR-XPS) at the free-electron laser FLASH. This novel experimental technique provides site-specific information about charge separation and enables the monitoring of free charge carrier generation dynamics on their natural timescale, here applied to the model donor-acceptor system CuPc:C60. A previously unobserved channel for exciton dissociation into mobile charge carriers is identified, providing the first direct, real-time characterization of the timescale and efficiency of charge generation from low-energy charge-transfer states in an organic heterojunction. The findings give strong support to the emerging realization that charge separation even from energetically disfavored excitonic states is contributing significantly, indicating new options for light harvesting in organic heterojunctions.

Date: 2021
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DOI: 10.1038/s41467-021-21454-3

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