RT Journal Article
T1 A Novel Pump-Pump-Probe Resonance Raman Approach Featuring Light-Induced Charge Accumulation on a Model Photosystem
A1 Cruz-Neto, Daniel H
A1 Soto-Martín, Juan
A1 Maity, Nishith
A1 Lefumeux, Christophe
A1 Nguyen, Thai
A1 Pernot, Pascal
A1 Steenkeste, Karine
A1 Peláez, Daniel
A1 Ha-Thi, M-H.
A1 Pino, Thomas
K1 Espectroscopía Raman
K1 Efecto Raman de resonancia
AB Light-induced charge accumulation is at the heart of biomimetic systems aiming at solar fuel production in the realm of artificial photosynthesis. Understanding the mechanisms upon which these processes operate is a necessary condition to drive down the rational catalyst design road. We have built a nanosecond pump-pump-probe resonance Raman setup to witness the sequential charge accumulation process while probing vibrational features of different charge- separated states. By employing a reversible model system featuring methyl viologen (MV) as dual electron acceptor, we have been able to watch the photosensitized production of its neutral form, MV0, resulting from two sequential electron transfer reactions. We have found that, upon double excitation, a fingerprint vibrational mode corresponding to the doubly reduced species appears at 992 cm-1 and peaks at 30 μs after the second excitation. This has been further confirmed by simulated resonance Raman spectra which fully support our experimental findings in this unprecedented build-up of charge seen by a resonance Raman probe.
PB American Chemical Society
YR 2023
FD 2023-05-15
LK https://hdl.handle.net/10630/46384
UL https://hdl.handle.net/10630/46384
LA eng
NO Cruz Neto, D. H., Soto, J., Maity, N., Lefumeux, C., Nguyen, T., Pernot, P., Steenkeste, K., Peláez, D., Ha-Thi, M.-H., & Pino, T. (2023). A Novel Pump–Pump–Probe Resonance Raman Approach Featuring Light-Induced Charge Accumulation on a Model Photosystem. The Journal of Physical Chemistry Letters, 14(20), 4789–4795. https://doi.org/10.1021/acs.jpclett.3c00594
DS RIUMA. Repositorio Institucional de la Universidad de Málaga
RD 13 may 2026