Coherent charge hopping suppresses photoexcited small polarons in ErFeO3 by antiadiabatic formation mechanism

Kim, Ye-Jin; Mendes, Jocelyn L.; Michelsen, Jonathan M.; Shin, Hyun Jun; Lee, Nara; Choi, Young Jai; Cushing, Scott K.

doi:10.1126/sciadv.adk4282

Coherent charge hopping suppresses photoexcited small polarons in ErFeO₃ by antiadiabatic formation mechanism

Journal Article · Wed Mar 20 00:00:00 EDT 2024 · Science Advances

DOI:https://doi.org/10.1126/sciadv.adk4282· OSTI ID:2471827

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California Institute of Technology (CalTech), Pasadena, CA (United States); California Inst. of Technology, Pasadena, CA (United States)
California Institute of Technology (CalTech), Pasadena, CA (United States)
Yonsei University, Seoul (Korea, Republic of)

Polarons are prevalent in condensed matter systems with strong electron-phonon coupling. The adiabaticity of the polaron relates to its transport properties and spatial extent. To date, only adiabatic small polaron formation has been measured following photoexcitation. The lattice reorganization energy is large enough that the first electron–optical phonon scattering event creates a small polaron without requiring substantial carrier thermalization. We measure that frustrating the iron-centered octahedra in the rare-earth orthoferrite ErFeO₃ leads to antiadiabatic polaron formation. Coherent charge hopping between neighboring Fe³⁺–Fe²⁺ sites is measured with transient extreme ultraviolet spectroscopy and lasts several picoseconds before the polaron forms. The resulting small polaron formation time is an order of magnitude longer than previous measurements and indicates a shallow potential well, even in the excited state. The results emphasize the importance of considering dynamic electron-electron correlations, not just electron-phonon–induced lattice changes, for small polarons for transport, catalysis, and photoexcited applications.

View Accepted Manuscript (DOE)

Research Organization:: California Institute of Technology (CalTech), Pasadena, CA (United States)

Sponsoring Organization:: USDOE Office of Science (SC), Basic Energy Sciences (BES); National Science Foundation Graduate Research Fellowship Program

Grant/Contract Number:: SC0021266

OSTI ID:: 2471827

Journal Information:: Science Advances, Journal Name: Science Advances Journal Issue: 12 Vol. 10; ISSN 2375-2548

Publisher:: AAASCopyright Statement

Country of Publication:: United States

Language:: English

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