Atomic-scale perspective of ultrafast charge transfer at a dye-semiconductor interface
Author(s)
Siefermann, KR
Pemmaraju, CD
Neppl, S
Shavorskiy, A
Cordones, AA
Vura-Weis, J
Slaughter, DS
Sturm, FP
Weise, F
Bluhm, H
Strader, ML
Cho, H
Lin, MF
Bacellar, C
Khurmi, C
Guo, J
Coslovich, G
Robinson, JS
Kaindl, RA
Schoenlein, RW
Belkacem, A
Neumark, DM
Leone, SR
Nordlund, D
Ogasawara, H
Krupin, O
Turner, JJ
Schlotter, WF
Holmes, MR
Messerschmidt, M
Minitti, MP
Gul, S
Zhang, JZ
Huse, N
Prendergast, D
Gessner, O
Griffith University Author(s)
Year published
2014
Metadata
Show full item recordAbstract
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 ᠰ.2) eV to higher binding ...
View more >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 ᠰ.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.
View less >
View more >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 ᠰ.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.
View less >
Journal Title
The Journal of Physical Chemistry Letters
Volume
5
Copyright Statement
Self-archiving of the author-manuscript version is not yet supported by this journal. Please refer to the journal link for access to the definitive, published version or contact the authors for more information.
Subject
Physical sciences
Chemical sciences