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  Evolution of hot polaron states with a nanosecond lifetime in a manganite perovskite.

Raiser, D., Mildner, S., Ifland, B., Sotoudeh, M., Blochl, P., Techert, S., et al. (2017). Evolution of hot polaron states with a nanosecond lifetime in a manganite perovskite. Advanced Energy Materials, 7(12): 1602174. doi:10.1002/aenm.201602174.

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Item Permalink: http://hdl.handle.net/11858/00-001M-0000-002D-9BC5-B Version Permalink: http://hdl.handle.net/11858/00-001M-0000-002D-9BCC-E
Genre: Journal Article

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Raiser, D.1, Author              
Mildner, S., Author
Ifland, B., Author
Sotoudeh, M., Author
Blochl, P., Author
Techert, S.1, Author              
Jooss, C., Author
Affiliations:
1Research Group of Structural Dynamics of (Bio)Chemical Systems, MPI for Biophysical Chemistry, Max Planck Society, ou_578564              

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 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.

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Language(s): eng - English
 Dates: 2017-01-242017-06-21
 Publication Status: Published in print
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 Rev. Method: Peer
 Identifiers: DOI: 10.1002/aenm.201602174
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Title: Advanced Energy Materials
Source Genre: Journal
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Pages: 10 Volume / Issue: 7 (12) Sequence Number: 1602174 Start / End Page: - Identifier: -