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.
Lan, Yang, et al. "Ultrafast correlated charge and lattice motion in a hybrid metal halide perovskite." Science Advances, vol. 5, no. 5, May. 2019. https://doi.org/10.1126/sciadv.aaw5558
Lan, Yang, Dringoli, Benjamin J., Valverde-Chávez, David A., Ponseca, Carlito S., Sutton, Mark, He, Yihui, Kanatzidis, Mercouri G., & Cooke, David G. (2019). Ultrafast correlated charge and lattice motion in a hybrid metal halide perovskite. Science Advances, 5(5). https://doi.org/10.1126/sciadv.aaw5558
Lan, Yang, Dringoli, Benjamin J., Valverde-Chávez, David A., et al., "Ultrafast correlated charge and lattice motion in a hybrid metal halide perovskite," Science Advances 5, no. 5 (2019), https://doi.org/10.1126/sciadv.aaw5558
@article{osti_1611842,
author = {Lan, Yang and Dringoli, Benjamin J. and Valverde-Chávez, David A. and Ponseca, Carlito S. and Sutton, Mark and He, Yihui and Kanatzidis, Mercouri G. and Cooke, David G.},
title = {Ultrafast correlated charge and lattice motion in a hybrid metal halide perovskite},
annote = {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.},
doi = {10.1126/sciadv.aaw5558},
url = {https://www.osti.gov/biblio/1611842},
journal = {Science Advances},
issn = {ISSN 2375-2548},
number = {5},
volume = {5},
place = {United States},
publisher = {AAAS},
year = {2019},
month = {05}}
LECTURE ON THE PHYSICS OF HIGHLY CORRELATED ELECTRON SYSTEMS VII: Seventh Training Course in the Physics of Correlated Electron Systems and High-Tc Superconductors, AIP Conference Proceedingshttps://doi.org/10.1063/1.1612391