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Title: Direct experimental evidence for photoinduced strong-coupling polarons in organolead halide perovskite nanoparticles

Journal Article · · Journal of Physical Chemistry Letters

Echoing the roaring success of their bulk coun-terparts, nano-objects built from organolead halide perov-skites (OLHP) present bright prospects for surpassing the performances of their conventional organic and inorganic analogues in photodriven technologies. Unraveling the pho-toinduced charge dynamics is essential for optimizing OLHP optoelectronic functionalities. However, mapping the carri-er-lattice interactions remains challenging, owing to their manifestations on multiple length scales and time scales. By correlating ultrafast time-resolved optical and X-ray absorp-tion measurements, this work reveals the photoinduced formation of strong-coupling polarons in CH3NH3PbBr3 nanoparticles. Such polarons originate from the self-trapping of electrons in the net Coulombic field caused by the dis-placed inorganic nuclei and the oriented organic cations. The transient structural change detected at the Pb L3 X-ray ab-sorption edge is well captured by a distortion with average bond elongation in the [PbBr6]2- motif. As a result, general implications for designing novel OLHP nanomaterials targeting the active utilization of these quasi-particles are outlined.

Research Organization:
Argonne National Laboratory (ANL), Argonne, IL (United States)
Sponsoring Organization:
USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22), Scientific User Facilities Division; Knut and Alice Wallenberg Foundation; Swedish Research Council (SRC)
Grant/Contract Number:
AC02-06CH11357
OSTI ID:
1369031
Journal Information:
Journal of Physical Chemistry Letters, Vol. 7, Issue 22; ISSN 1948-7185
Publisher:
American Chemical SocietyCopyright Statement
Country of Publication:
United States
Language:
English
Citation Metrics:
Cited by: 44 works
Citation information provided by
Web of Science

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Cited By (13)

Barrier to recombination of oppositely charged large polarons journal February 2018
Properties of Excitons and Photogenerated Charge Carriers in Metal Halide Perovskites journal September 2018
Proposed high-power beta cells from MgAlB 14 -type icosahedral-boron semiconductors journal May 2019
Crystal structures and rotational dynamics of a two-dimensional metal halide perovskite (OA) 2 PbI 4 journal January 2020
Direct Observation of Halide Migration and its Effect on the Photoluminescence of Methylammonium Lead Bromide Perovskite Single Crystals journal September 2017
Polarons in Metal Halide Perovskites journal April 2020
Hot Polarons with Trapped Excitons and Octahedra‐Twist Phonons in CH 3 NH 3 PbBr 3 Hybrid Perovskite Nanowires journal November 2019
Large polarons in lead halide perovskites journal August 2017
Large polaron formation and its effect on electron transport in hybrid perovskites journal January 2019
Light-induced lattice expansion leads to high-efficiency perovskite solar cells journal April 2018
Large (bi)Polarons for Novel Energy Conversion and Superconductivity journal October 2019
Hot Polarons with Trapped Excitons and Octahedra-Twist Phonons in CH3NH3PbBr3 Hybrid Perovskite Nanowires text January 2019
Photoexcitation Dynamics in Electrochemically Charged CdSe Quantum Dots: From Hot Carrier Cooling to Auger Recombination of Negative Trions journal December 2020

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