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

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.

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Item Permalink: http://hdl.handle.net/11858/00-001M-0000-0024-B282-5 Version Permalink: http://hdl.handle.net/11858/00-001M-0000-0026-B2E4-0
Genre: Journal Article

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http://dx.doi.org/10.1021/jz501264x (Publisher version)
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 Creators:
Siefermann, Katrin R., Author
Pemmaraju, Chaitanya D., Author
Neppl, Stefan, Author
Shavorskiy, Andrey, Author
Cordones, Amy A., Author
Vura-Weis, Josh, Author
Slaughter, Daniel S., Author
Sturm, Felix P., Author
Weise, Fabian, Author
Bluhm, Hendrik, Author
Strader, Matthew L., Author
Cho, Hana, Author
Lin, Ming-Fu, Author
Bacellar, Camila, Author
Khurmi, Champak, Author
Guo, Jinghua, Author
Coslovich, Giacomo, Author
Robinson, Joseph S., Author
Kaindl, Robert A., Author
Schoenlein, Robert W., Author
Belkacem, Ali, AuthorNeumark, Daniel M., AuthorLeone, Stephen R., AuthorNordlund, Dennis, AuthorOgasawara, Hirohito, AuthorKrupin, Oleg, AuthorTurner, Joshua J., AuthorSchlotter, William F., AuthorHolmes, Michael R., AuthorMesserschmidt, Marc, AuthorMinitti, Michael P., AuthorGul, Sheraz, AuthorZhang, Jin Z., AuthorHuse, Nils1, 2, Author              Prendergast, David, AuthorGessner, Oliver, Author more..
Affiliations:
1Ultrafast Molecular Dynamics, Atomically Resolved Dynamics Department, Max Planck Institute for the Structure and Dynamics of Matter, Max Planck Society, ou_1938289              
2University of Hamburg, External Organizations, ou_2035287              

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Free keywords: Spectroscopy; Photochemistry; Excited States
 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.

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Language(s): eng - English
 Dates: 2014-06-202014-07-252014-07-252014-08-07
 Publication Status: Published in print
 Pages: 7
 Publishing info: -
 Table of Contents: -
 Rev. Method: Peer
 Identifiers: DOI: 10.1021/jz501264x
 Degree: -

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Title: The Journal of Physical Chemistry Letters
Source Genre: Journal
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Affiliations:
Publ. Info: -
Pages: - Volume / Issue: 5 (15) Sequence Number: - Start / End Page: 2753 - 2759 Identifier: -