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Impact of Crystallographic Orientation Disorders on Electronic Heterogeneities in Metal Halide Perovskite Thin Films

Journal Article · · Nano Letters
Metal halide perovskite thin films have achieved remarkable performance in optoelectronic devices. To achieve higher device performance and reliability needed for wide-spread commercial deployment, spatial heterogeneity of optoelectronic properties in the perovskite thin films needs to be understood and controlled. However, clear identification of the causes underlying the heterogeneity has remained elusive. In this work, we employ a multimodal imaging approach to separate electronic heterogeneity from morphology variations in perovskite thin films. Our results reveal that disorders in the crystallographic orientation of grains and different surface terminations are the primary cause of the electronic heterogeneity. Therefore, a solution processed polycrystalline perovskite thin film with a negligible spatial variation in charge trap site density reaching that of single crystals can be achieved by minimizing crystallographic orientation disorder.
Research Organization:
Oak Ridge National Laboratory (ORNL), Oak Ridge, TN (United States)
Sponsoring Organization:
National Science Foundation (NSF); USDOE Office of Science (SC), Basic Energy Sciences (BES). Chemical Sciences, Geosciences & Biosciences Division
Grant/Contract Number:
AC05-00OR22725; SC0016144
OSTI ID:
1784202
Journal Information:
Nano Letters, Journal Name: Nano Letters Journal Issue: 10 Vol. 18; ISSN 1530-6984
Publisher:
American Chemical SocietyCopyright Statement
Country of Publication:
United States
Language:
English

References (50)

Impact of Crystal Surface on Photoexcited States in Organic-Inorganic Perovskites journal December 2016
High Charge Carrier Mobilities and Lifetimes in Organolead Trihalide Perovskites journal December 2013
Square-Centimeter Solution-Processed Planar CH 3 NH 3 PbI 3 Perovskite Solar Cells with Efficiency Exceeding 15% journal September 2015
Local Versus Long-Range Diffusion Effects of Photoexcited States on Radiative Recombination in Organic-Inorganic Lead Halide Perovskites journal July 2015
Nanoimaging of Open-Circuit Voltage in Photovoltaic Devices journal September 2015
Identifying the Real Minority Carrier Lifetime in Nonideal Semiconductors: A Case Study of Kesterite Materials journal May 2017
Methylamine-Gas-Induced Defect-Healing Behavior of CH 3 NH 3 PbI 3 Thin Films for Perovskite Solar Cells journal June 2015
Limiting Perovskite Solar Cell Performance by Heterogeneous Carrier Extraction journal October 2016
Perovskite Solar Cells: From the Atomic Level to Film Quality and Device Performance journal February 2018
Metal Halide Perovskite Polycrystalline Films Exhibiting Properties of Single Crystals journal September 2017
Photoconductive noise microscopy revealing quantitative effect of localized electronic traps on the perovskite-based solar cell performance journal January 2018
Hybrid Perovskites for Photovoltaics: Charge-Carrier Recombination, Diffusion, and Radiative Efficiencies journal December 2015
Spatially Heterogeneous Chlorine Incorporation in Organic–Inorganic Perovskite Solar Cells journal September 2016
Charge Carriers in Planar and Meso-Structured Organic–Inorganic Perovskites: Mobilities, Lifetimes, and Concentrations of Trap States journal July 2015
Organometal Trihalide Perovskite Single Crystals: A Next Wave of Materials for 25% Efficiency Photovoltaics and Applications Beyond? journal July 2015
Spatially Non-uniform Trap State Densities in Solution-Processed Hybrid Perovskite Thin Films journal February 2016
Approaching Bulk Carrier Dynamics in Organo-Halide Perovskite Nanocrystalline Films by Surface Passivation journal March 2016
Imaging Electronic Trap States in Perovskite Thin Films with Combined Fluorescence and Femtosecond Transient Absorption Microscopy journal April 2016
Charge Carrier Trapping at Surface Defects of Perovskite Solar Cell Absorbers: A First-Principles Study journal January 2017
Separating Bulk and Surface Contributions to Electronic Excited-State Processes in Hybrid Mixed Perovskite Thin Films via Multimodal All-Optical Imaging journal July 2017
Mapping the Photoresponse of CH 3 NH 3 PbI 3 Hybrid Perovskite Thin Films at the Nanoscale journal May 2016
Double Charged Surface Layers in Lead Halide Perovskite Crystals journal February 2017
Real-Time Nanoscale Open-Circuit Voltage Dynamics of Perovskite Solar Cells journal March 2017
Facet-Dependent Property of Sequentially Deposited Perovskite Thin Films: Chemical Origin and Self-Annihilation journal November 2016
Photoluminescence Lifetimes Exceeding 8 μs and Quantum Yields Exceeding 30% in Hybrid Perovskite Thin Films by Ligand Passivation journal July 2016
Photovoltage Tomography in Polycrystalline Solar Cells journal October 2016
Gas-Induced Formation/Transformation of Organic–Inorganic Halide Perovskites journal August 2017
Anticorrelation between Local Photoluminescence and Photocurrent Suggests Variability in Contact to Active Layer in Perovskite Solar Cells journal October 2016
Tracking Photoexcited Carriers in Hybrid Perovskite Semiconductors: Trap-Dominated Spatial Heterogeneity and Diffusion journal September 2017
Separation of Distinct Photoexcitation Species in Femtosecond Transient Absorption Microscopy journal February 2016
Controlling Nanocrystal Superlattice Symmetry and Shape-Anisotropic Interactions through Variable Ligand Surface Coverage journal March 2011
Interface-Induced Nucleation, Orientational Alignment and Symmetry Transformations in Nanocube Superlattices journal January 2012
Nanoscale Imaging of Photocurrent and Efficiency in CdTe Solar Cells journal October 2014
Enhanced optoelectronic quality of perovskite thin films with hypophosphorous acid for planar heterojunction solar cells journal November 2015
Spatial and temporal imaging of long-range charge transport in perovskite thin films by ultrafast microscopy journal June 2015
Low surface recombination velocity in solution-grown CH3NH3PbBr3 perovskite single crystal journal August 2015
Perovskite solar cells: Different facets of performance journal July 2016
Towards stable and commercially available perovskite solar cells journal October 2016
Top and bottom surfaces limit carrier lifetime in lead iodide perovskite films journal January 2017
Facet-dependent photovoltaic efficiency variations in single grains of hybrid halide perovskite journal July 2016
Origin of vertical orientation in two-dimensional metal halide perovskites and its effect on photovoltaic performance journal April 2018
Analysing the effect of crystal size and structure in highly efficient CH 3 NH 3 PbI 3 perovskite solar cells by spatially resolved photo- and electroluminescence imaging journal January 2015
Thermally induced recrystallization of MAPbI 3 perovskite under methylamine atmosphere: an approach to fabricating large uniform crystalline grains journal January 2016
Do grain boundaries dominate non-radiative recombination in CH 3 NH 3 PbI 3 perovskite thin films? journal January 2017
Quantification of spatial inhomogeneity in perovskite solar cells by hyperspectral luminescence imaging journal January 2016
The rapid evolution of highly efficient perovskite solar cells journal January 2017
Controlling nucleation, growth, and orientation of metal halide perovskite thin films with rationally selected additives journal January 2017
A quantitative and spatially resolved analysis of the performance-bottleneck in high efficiency, planar hybrid perovskite solar cells journal January 2018
Crystallographic orientation propagation in metal halide perovskite thin films journal January 2017
Impact of microstructure on local carrier lifetime in perovskite solar cells journal April 2015

Cited By (3)

The Impact of Stoichiometry on the Photophysical Properties of Ruddlesden–Popper Perovskites journal November 2019
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
Effect of density of surface defects on photoluminescence properties in MAPbI 3 perovskite films journal January 2019

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