Ultrafast correlated charge and lattice motion in a hybrid metal halide perovskite

Abstract

Hybrid organic-inorganic halide perovskites have shown remarkable optoelectronic properties (1-3), believed to originate from correlated motion of charge carriers and the polar lattice forming large polarons (4-7). Few experimental techniques are capable of probing these correlations directly, requiring simultaneous sub-meV energy and femtosecond temporal resolution after absorption of a photon (8). Here we use transient multi-THz spectroscopy, sensitive to the internal motions of charges within 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 quantum beats arising from the coherent displacement of charge from the coupled phonon cloud. Our measurements provide unambiguous evidence of the existence of polarons in MAPI.

References in corpus (5)

• Local polar fluctuations in lead halide perovskite crystals
• Phonon coherences reveal the polaronic character of excitons in two-dimensional lead-halide perovskites
• Intrinsic femtosecond charge generation dynamics in a single crystal organometal halide perovskite
• Probing Femtosecond Lattice Displacement upon Photo-carrier generation in Lead Halide Perovskite
• Carrier Lifetimes and Polaronic Mass Enhancement in the Hybrid Halide Perovskite CH${}_3$NH${}_3$PbI${}_3$ from Multiphonon Fröhlich Coupling

Cited by in corpus (1)

• Perspective: Exciton polarons in two-dimensional hybrid metal-halide perovskites