Evolution of Hot Polaron States with a Nanosecond Lifetime in a Manganite Perovskite
2017-06-21 | journal article; research paper. A publication with affiliation to the University of Göttingen.
Jump to: Cite & Linked | Documents & Media | Details | Version history
Cite this publication
Evolution of Hot Polaron States with a Nanosecond Lifetime in a Manganite Perovskite
Raiser, D. ; Mildner, S. ; Ifland, B. ; Sotoudeh, M.; Bloechl, P. E.; Techert, S. & Jooss, C. (2017)
Advanced Energy Materials, 7(12) art. 1602174. DOI: https://doi.org/10.1002/aenm.201602174
Documents & Media
Details
- Authors
- Raiser, Dirk ; Mildner, Stephanie ; Ifland, Benedikt ; Sotoudeh, Mohsen; Bloechl, Peter E.; Techert, Simone ; Jooss, Christian
- Abstract
- Understanding and controlling the relaxation process of optically excited charge carriers in solids with strong correlations is of great interest in the quest for new strategies to exploit solar energy. Usually, optically excited electrons in a solid thermalize rapidly on a femtosecond to picosecond timescale due to interactions with other electrons and phonons. New mechanisms to slow down thermalization will thus be of great significance for efficient light energy conversion, e.g., in photovoltaic devices. Ultrafast optical pump-probe experiments in the manganite Pr0.65Ca0.35MnO3, a photovoltaic, thermoelectric, and electrocatalytic material with strong polaronic correlations, reveal an ultraslow recombination dynamics on a nanosecond-time scale. The nature of long living excitations is further elucidated by photovoltaic measurements, showing the presence of photodiffusion of excited electron-hole polaron pairs. Theoretical considerations suggest that the excited charge carriers are trapped in a hot polaron state. Escape from this state is possible via a slow dipole-forbidden recombination process or via rare thermal fluctuations toward a conical intersection followed by a radiation-less decay. The strong correlation between the excited polaron and the octahedral dynamics of its environment appears to be substantial for stabilizing the hot polaron.
- Issue Date
- 21-June-2017
- Journal
- Advanced Energy Materials
- Project
- SFB 1073: Kontrolle von Energiewandlung auf atomaren Skalen
SFB 1073 | Topical Area B | B02 Photonen-getriebener Energietransfer über Grenzflächen zwischen Materialien mit starken Korrelationen
SFB 1073 | Topical Area B | B03 Relaxation, Thermalisierung, Transport und Kondensation in hochangeregten Festkörpern
SFB 1073 | Topical Area C | C02 In situ hochauflösende Untersuchung des aktiven Zustands bei der photo- und elektrochemischen Wasserspaltung
SFB 1073 | Topical Area C | C03 Vom Elektronentransfer zur chemischen Energiespeicherung: ab-initio Untersuchungen korrelierter Prozesse - Organization
- Institut für Materialphysik ; Institut für Röntgenphysik
- Working Group
- RG Techert (Structural Dynamics in Chemical Systems)
- ISSN
- 1614-6840; 1614-6832
- Language
- English
- Sponsor
- Deutsche Forschungsgemeinschaft (DFG) [CRC 1073, CRC 755]