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Title: Spatial localization of excitons and charge carriers in hybrid perovskite thin films

Journal Article · · Journal of Physical Chemistry Letters

The fundamental photophysics underlying the remarkably high power conversion efficiency of organic-inorganic hybrid perovskite-based solar cells has been increasingly studied using complementary spectroscopic techniques. The spatially heterogeneous polycrystalline morphology of the photoactive layers owing to the presence of distinct crystalline grains has been generally neglected in optical measurements and therefore the reported results are typically averaged over hundreds or even thousands of such grains. Here, we apply femtosecond transient absorption microscopy to spatially and temporally probe ultrafast electronic excited-state dynamics in pristine methylammonium lead tri-iodide (CH3NH3PbI3) thin films and composite structures. We found that the electronic excited-state relaxation kinetics are extremely sensitive to the sample location probed, which was manifested by position-dependent decay timescales and transient signals. As a result, analysis of transient absorption kinetics acquired at distinct spatial positions enabled us to identify contributions of excitons and free charge carriers.

Research Organization:
Oak Ridge National Laboratory (ORNL), Oak Ridge, TN (United States)
Sponsoring Organization:
USDOE Office of Science (SC), Basic Energy Sciences (BES)
Grant/Contract Number:
AC05-00OR22725
OSTI ID:
1209208
Journal Information:
Journal of Physical Chemistry Letters, Vol. 6, Issue 15; ISSN 1948-7185
Publisher:
American Chemical SocietyCopyright Statement
Country of Publication:
United States
Language:
English
Citation Metrics:
Cited by: 56 works
Citation information provided by
Web of Science

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Cited By (18)

How Methylammonium Cations and Chlorine Dopants Heal Defects in Lead Iodide Perovskites journal January 2018
Twin domains modulate light-matter interactions in metal halide perovskites journal January 2020
Properties of Excitons and Photogenerated Charge Carriers in Metal Halide Perovskites journal September 2018
Perovskite Excitonics: Primary Exciton Creation and Crossover from Free Carriers to a Secondary Exciton Phase journal December 2017
Compressed supercontinuum probe for transient absorption microscopy journal January 2018
Invited Review Article: Pump-probe microscopy journal March 2016
Transient absorption microscopy: Technological innovations and applications in materials science and life science journal January 2020
Compressive imaging of transient absorption dynamics on the femtosecond timescale journal January 2019
Three applications of ultrafast transient absorption spectroscopy of semiconductor thin films: spectroelectrochemistry, microscopy, and identification of thermal contributions journal January 2018
Ultrafast measurements of the dynamics of single nanostructures: a review journal November 2018
Heterogeneity at multiple length scales in halide perovskite semiconductors journal July 2019
Spatially segregated free-carrier and exciton populations in individual lead halide perovskite grains journal March 2017
Probing the Spatial Heterogeneity of Carrier Relaxation Dynamics in CH 3 NH 3 PbI 3 Perovskite Thin Films with Femtosecond Time‐Resolved Nonlinear Optical Microscopy journal August 2019
Edge Effect on the Population of Free Carriers and Excitons in Single‐Crystal CH 3 NH 3 PbBr 3 Perovskite Nanomaterials journal May 2019
How Methylammonium Cations and Chlorine Dopants Heal Defects in Lead Iodide Perovskites journalarticle January 2018
Heterogeneity at multiple length scales in halide perovskite semiconductors text January 2019
Compressive imaging of transient absorption dynamics on the femtosecond timescale text January 2019
Exciton Relaxation Dynamics in Photo-Excited CsPbI3 Perovskite Nanocrystals journal July 2016