skip to main content
OSTI.GOV title logo U.S. Department of Energy
Office of Scientific and Technical Information

Title: Direct Correlation of Charge Carrier Transport to Local Crystal Quality in Lead Halide Perovskites

Journal Article · · Nano Letters

Although solution processing methods provide an attractive route toward development of low-cost functional materials, these accessible fabrication approaches can engender high concentrations of microscopic structural defects that are detrimental to performance. In lead halide perovskites, structural disorder derived from solution processing has been implicated as an important determiner of photophysical properties. However, a direct correlation between the functional properties of these materials and the local crystal structure in which non-equilibrium states evolve has remained elusive, in part because structural heterogeneities occur on length scales that defy conventional characterization techniques. To address this knowledge gap, in this work we have combined ultrafast pump–probe microscopy and electron backscattering diffraction to directly correlate charge carrier transport with the local diffraction pattern contrast, an indicator of crystal quality. Spatial correlation of these measurements strongly suggests that even on individual single crystal CsPbBr3 domains, microscopic variability in the crystal quality profoundly impacts the efficiency of charge carrier transport.

Research Organization:
Montana State Univ., Bozeman, MT (United States)
Sponsoring Organization:
USDOE Office of Science (SC), Basic Energy Sciences (BES). Chemical Sciences, Geosciences & Biosciences Division; Beckman Young Investigator Program; National Science Foundation (NSF)
Grant/Contract Number:
SC0014128; 1632134
OSTI ID:
1658903
Journal Information:
Nano Letters, Vol. 20, Issue 7; ISSN 1530-6984
Publisher:
American Chemical SocietyCopyright Statement
Country of Publication:
United States
Language:
English
Citation Metrics:
Cited by: 8 works
Citation information provided by
Web of Science

References (47)

Controlling Thin-Film Stress and Wrinkling during Perovskite Film Formation journal May 2018
Relationships between Lead Halide Perovskite Thin-Film Fabrication, Morphology, and Performance in Solar Cells journal November 2015
Influence of structural defects in solution-processed InZnO semiconductors on the electrical stability of thin-film transistors journal December 2016
Ultra-high mobility transparent organic thin film transistors grown by an off-centre spin-coating method journal January 2014
Air-Exposure Induced Dopant Redistribution and Energy Level Shifts in Spin-Coated Spiro-MeOTAD Films journal January 2015
Instilling defect tolerance in new compounds journal September 2017
Impact of non-equilibrium molecular packings on singlet fission in microcrystals observed using 2D white-light microscopy journal December 2019
Exciton dynamics reveal aggregates with intermolecular order at hidden interfaces in solution-cast organic semiconducting films journal January 2015
New Strategies for Defect Passivation in High‐Efficiency Perovskite Solar Cells journal April 2020
Strain engineering in perovskite solar cells and its impacts on carrier dynamics journal February 2019
Terahertz Conductivity within Colloidal CsPbBr 3 Perovskite Nanocrystals: Remarkably High Carrier Mobilities and Large Diffusion Lengths journal July 2016
Screening Links Transport and Recombination Mechanisms in Lead Halide Perovskites journal June 2019
Centimeter-Sized Inorganic Lead Halide Perovskite CsPbBr 3 Crystals Grown by an Improved Solution Method journal October 2017
Large polarons in lead halide perovskites journal August 2017
Air-stable CsPb 1−x Bi x Br 3 (0 ≤ x ≪ 1) perovskite crystals: optoelectronic and photostriction properties journal January 2017
Inorganic Lead Halide Perovskite Single Crystals: Phase-Selective Low-Temperature Growth, Carrier Transport Properties, and Self-Powered Photodetection journal December 2016
Direct Measurements of Carrier Transport in Polycrystalline Methylammonium Lead Iodide Perovskite Films with Transient Grating Spectroscopy journal September 2018
Anisotropy of Thermal Diffusivity in Lead Halide Perovskite Layers Revealed by Thermal Grating Technique journal May 2019
Photovoltaic mixed-cation lead mixed-halide perovskites: links between crystallinity, photo-stability and electronic properties journal January 2017
Grain-Size-Limited Mobility in Methylammonium Lead Iodide Perovskite Thin Films journal August 2016
Transient Sub-Band-Gap States at Grain Boundaries of CH 3 NH 3 PbI 3 Perovskite Act as Fast Temperature Relaxation Centers journal June 2019
Ultrafast Imaging of Carrier Transport across Grain Boundaries in Hybrid Perovskite Thin Films journal May 2018
Imaging material functionality through three-dimensional nanoscale tracking of energy flow journal October 2019
Subgrain Special Boundaries in Halide Perovskite Thin Films Restrict Carrier Diffusion journal October 2018
Tracking Photoexcited Carriers in Hybrid Perovskite Semiconductors: Trap-Dominated Spatial Heterogeneity and Diffusion journal September 2017
Do grain boundaries dominate non-radiative recombination in CH 3 NH 3 PbI 3 perovskite thin films? journal January 2017
Lattice strain causes non-radiative losses in halide perovskites journal January 2019
Ultrafast Excited-State Transport and Decay Dynamics in Cesium Lead Mixed Halide Perovskites journal June 2017
Ambipolar diffusion of photoexcited carriers in bulk GaAs journal December 2010
Reduced Artifact Approach for Determining Diffusion Coefficients in Time-Resolved Microscopy journal May 2020
Tutorial: Crystal orientations and EBSD — Or which way is up? journal July 2016
Impact of Reabsorption on the Emission Spectra and Recombination Dynamics of Hybrid Perovskite Single Crystals journal June 2017
EBSD Image Quality Mapping journal December 2005
Image Quality Analysis: A New Method of Characterizing Microstructures journal January 2005
A Review of Strain Analysis Using Electron Backscatter Diffraction journal March 2011
Errors, Artifacts, and Improvements in EBSD Processing and Mapping journal January 2005
Hough Transform from the Radon Transform journal March 1981
Electron Backscatter Diffraction in Materials Science book January 2009
Perovskite Carrier Transport: Disentangling the Impacts of Effective Mass and Scattering Time Through Microscopic Optical Detection journal May 2018
Film stresses and electrode buckling in organic solar cells journal August 2012
Strained hybrid perovskite thin films and their impact on the intrinsic stability of perovskite solar cells journal November 2017
Defects in perovskite-halides and their effects in solar cells journal October 2016
Using SMILES strings for the description of chemical connectivity in the Crystallography Open Database journal May 2018
Crystallography Open Database – an open-access collection of crystal structures journal May 2009
Crystallography Open Database (COD): an open-access collection of crystal structures and platform for world-wide collaboration journal November 2011
Computing stoichiometric molecular composition from crystal structures journal January 2015
COD::CIF::Parser : an error-correcting CIF parser for the Perl language journal February 2016