Atomic-Scale Perspective of Ultrafast Charge Transfer at a Dye–Semiconductor 
Interface

Siefermann, Katrin R.; Pemmaraju, Chaitanya D.; Neppl, Stefan; Shavorskiy, Andrey; Cordones, Amy A.; Vura-Weis, Josh; Slaughter, Daniel S.; Sturm, Felix P.; Weise, Fabian; Bluhm, Hendrik; Strader, Matthew L.; Cho, Hana; Lin, Ming-Fu; Bacellar, Camila; Khurmi, Champak; Guo, Jinghua; Coslovich, Giacomo; Robinson, Joseph S.; Kaindl, Robert A.; Schoenlein, Robert W.; Belkacem, Ali; Neumark, Daniel M.; Leone, Stephen R.; Nordlund, Dennis; Ogasawara, Hirohito; Krupin, Oleg; Turner, Joshua J.; Schlotter, William F.; Holmes, Michael R.; Messerschmidt, Marc; Minitti, Michael P.; Gul, Sheraz; Zhang, Jin Z.; Huse, Nils; Prendergast, David; Gessner, Oliver

doi:10.1021/jz501264x

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Atomic-Scale Perspective of Ultrafast Charge Transfer at a Dye–Semiconductor Interface

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Huse, Nils
Ultrafast Molecular Dynamics, Atomically Resolved Dynamics Department, Max Planck Institute for the Structure and Dynamics of Matter, Max Planck Society;
University of Hamburg, External Organizations;

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http://dx.doi.org/10.1021/jz501264x
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Citation

Siefermann, K. R., Pemmaraju, C. D., Neppl, S., Shavorskiy, A., Cordones, A. A., Vura-Weis, J., et al. (2014). Atomic-Scale Perspective of Ultrafast Charge Transfer at a Dye–Semiconductor Interface. The Journal of Physical Chemistry Letters, 5(15), 2753-2759. doi:10.1021/jz501264x.

Cite as: https://hdl.handle.net/11858/00-001M-0000-0024-B282-5

Abstract

Understanding interfacial charge-transfer processes on the atomic level is crucial to support the rational design of energy-challenge relevant systems such as solar cells, batteries, and photocatalysts. A femtosecond time-resolved core-level photoelectron spectroscopy study is performed that probes the electronic structure of the interface between ruthenium-based N3 dye molecules and ZnO nanocrystals within the first picosecond after photoexcitation and from the unique perspective of the Ru reporter atom at the center of the dye. A transient chemical shift of the Ru 3d inner-shell photolines by (2.3 ± 0.2) eV to higher binding energies is observed 500 fs after photoexcitation of the dye. The experimental results are interpreted with the aid of ab initio calculations using constrained density functional theory. Strong indications for the formation of an interfacial charge-transfer state are presented, providing direct insight into a transient electronic configuration that may limit the efficiency of photoinduced free charge-carrier generation.