Abstract:
:Hybrid organic-inorganic halide perovskites have shown remarkable optoelectronic properties, exhibiting an impressive tolerance to defects believed to originate from correlated motion of charge carriers and the polar lattice forming large polarons. Few experimental techniques are capable of directly probing these correlations, requiring simultaneous sub-millielectron volt energy and femtosecond temporal resolution after absorption of a photon. Here, we use time-resolved multi-THz spectroscopy, sensitive to the internal excitations of the polaron, to temporally and energetically resolve the coherent coupling of charges to longitudinal optical phonons in single-crystal CH3NH3PbI3 (MAPI). We observe room temperature intraband quantum beats arising from the coherent displacement of charge from the coupled phonon cloud. Our measurements provide strong evidence for the existence of polarons in MAPI at room temperature, suggesting that electron/hole-phonon coupling is a defining aspect of the hybrid metal-halide perovskites contributing to the protection from scattering and enhanced carrier lifetimes that define their usefulness in devices.
journal_name
Sci Advjournal_title
Science advancesauthors
Lan Y,Dringoli BJ,Valverde-Chávez DA,Ponseca CS Jr,Sutton M,He Y,Kanatzidis MG,Cooke DGdoi
10.1126/sciadv.aaw5558subject
Has Abstractpub_date
2019-05-31 00:00:00pages
eaaw5558issue
5issn
2375-2548pii
aaw5558journal_volume
5pub_type
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