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Title: Grain boundary dominated ion migration in polycrystalline organic–inorganic halide perovskite films

Abstract

The efficiency of perovskite solar cells is approaching that of single-crystalline silicon solar cells despite the presence of large grain boundary (GB) area in the polycrystalline thin films. Here, by using a combination of nanoscopic and macroscopic level measurements, we show that the ion migration in polycrystalline perovskites is dominated through GBs. Conducting atomic force microscopy measurements reveal much stronger hysteresis both for photocurrent and dark-current at the GBs than on the grains interiors, which can be explained by faster ion migration at the GBs. The dramatically enhanced ion migration results in a redistribution of ions along the GBs after electric poling, in contrast to the intact grain area. The perovskite single-crystal devices without GBs show negligible current hysteresis and no ion-migration signal. Furthermore, the discovery of dominating ion migration through GBs in perovskites can lead to broad applications in many types of devices including photovoltaics, memristors, and ion batteries.

Authors:
 [1];  [1];  [1];  [1];  [1];  [1];  [1];  [1];  [1];  [1];  [1];  [1]
  1. Univ. of Nebraska-Lincoln, Lincoln, NE (United States)
Publication Date:
Research Org.:
Univ. of Nebraska, Lincoln, NE (United States)
Sponsoring Org.:
USDOE Office of Energy Efficiency and Renewable Energy (EERE), Renewable Power Office. Solar Energy Technologies Office
OSTI Identifier:
1342745
Grant/Contract Number:  
EE0006709
Resource Type:
Accepted Manuscript
Journal Name:
Energy & Environmental Science
Additional Journal Information:
Journal Volume: 9; Journal Issue: 5; Journal ID: ISSN 1754-5692
Publisher:
Royal Society of Chemistry
Country of Publication:
United States
Language:
English
Subject:
36 MATERIALS SCIENCE; 14 SOLAR ENERGY

Citation Formats

Shao, Yuchuan, Fang, Yanjun, Li, Tao, Wang, Qi, Dong, Qingfeng, Deng, Yehao, Yuan, Yongbo, Wei, Haotong, Wang, Meiyu, Gruverman, Alexei, Shield, Jeffery, and Huang, Jinsong. Grain boundary dominated ion migration in polycrystalline organic–inorganic halide perovskite films. United States: N. p., 2016. Web. doi:10.1039/C6EE00413J.
Shao, Yuchuan, Fang, Yanjun, Li, Tao, Wang, Qi, Dong, Qingfeng, Deng, Yehao, Yuan, Yongbo, Wei, Haotong, Wang, Meiyu, Gruverman, Alexei, Shield, Jeffery, & Huang, Jinsong. Grain boundary dominated ion migration in polycrystalline organic–inorganic halide perovskite films. United States. https://doi.org/10.1039/C6EE00413J
Shao, Yuchuan, Fang, Yanjun, Li, Tao, Wang, Qi, Dong, Qingfeng, Deng, Yehao, Yuan, Yongbo, Wei, Haotong, Wang, Meiyu, Gruverman, Alexei, Shield, Jeffery, and Huang, Jinsong. Mon . "Grain boundary dominated ion migration in polycrystalline organic–inorganic halide perovskite films". United States. https://doi.org/10.1039/C6EE00413J. https://www.osti.gov/servlets/purl/1342745.
@article{osti_1342745,
title = {Grain boundary dominated ion migration in polycrystalline organic–inorganic halide perovskite films},
author = {Shao, Yuchuan and Fang, Yanjun and Li, Tao and Wang, Qi and Dong, Qingfeng and Deng, Yehao and Yuan, Yongbo and Wei, Haotong and Wang, Meiyu and Gruverman, Alexei and Shield, Jeffery and Huang, Jinsong},
abstractNote = {The efficiency of perovskite solar cells is approaching that of single-crystalline silicon solar cells despite the presence of large grain boundary (GB) area in the polycrystalline thin films. Here, by using a combination of nanoscopic and macroscopic level measurements, we show that the ion migration in polycrystalline perovskites is dominated through GBs. Conducting atomic force microscopy measurements reveal much stronger hysteresis both for photocurrent and dark-current at the GBs than on the grains interiors, which can be explained by faster ion migration at the GBs. The dramatically enhanced ion migration results in a redistribution of ions along the GBs after electric poling, in contrast to the intact grain area. The perovskite single-crystal devices without GBs show negligible current hysteresis and no ion-migration signal. Furthermore, the discovery of dominating ion migration through GBs in perovskites can lead to broad applications in many types of devices including photovoltaics, memristors, and ion batteries.},
doi = {10.1039/C6EE00413J},
journal = {Energy & Environmental Science},
number = 5,
volume = 9,
place = {United States},
year = {Mon Mar 21 00:00:00 EDT 2016},
month = {Mon Mar 21 00:00:00 EDT 2016}
}

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journal, January 2019

  • Petrović, Miloš; Maksudov, Temur; Panagiotopoulos, Apostolos
  • Nanoscale Advances, Vol. 1, Issue 8
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Furrowed hole-transport layer using argon plasma in an inverted perovskite solar cell
journal, January 2019

  • Li, Xiao-Mei; Wang, Kai-li; Jiang, Yu-Rong
  • New Journal of Chemistry, Vol. 43, Issue 36
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A polyaspartic acid sodium interfacial layer enhances surface trap passivation in perovskite solar cells
journal, January 2019

  • Wang, Boxin; Wu, Fei; Bi, Shiqing
  • Journal of Materials Chemistry A, Vol. 7, Issue 41
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Sulfonyl-based non-fullerene electron acceptor-assisted grain boundary passivation for efficient and stable perovskite solar cells
journal, January 2019

  • Song, Changjian; Li, Xiaodong; Wang, Yueming
  • Journal of Materials Chemistry A, Vol. 7, Issue 34
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Perspective: Theory and simulation of hybrid halide perovskites
journal, June 2017

  • Whalley, Lucy D.; Frost, Jarvist M.; Jung, Young-Kwang
  • The Journal of Chemical Physics, Vol. 146, Issue 22
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The investigation of the unseen interrelationship of grain size, ionic defects, device physics and performance of perovskite solar cells
journal, January 2019

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  • Journal of Physics D: Applied Physics, Vol. 52, Issue 12
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Inverted hysteresis in MAPbI 3 perovskite solar cells induced by presetting bias voltage
journal, May 2019

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  • Journal of Physics D: Applied Physics, Vol. 52, Issue 31
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Operational stability of perovskite light emitting diodes
journal, January 2020


Understanding charge transport in lead iodide perovskite thin-film field-effect transistors
journal, January 2017

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Polymer-modified halide perovskite films for efficient and stable planar heterojunction solar cells
journal, August 2017


Stabilizing halide perovskite surfaces for solar cell operation with wide-bandgap lead oxysalts
journal, August 2019


Composition-Tuned Wide Bandgap Perovskites: From Grain Engineering to Stability and Performance Improvement
journal, July 2018

  • Zhou, Yang; Jia, Yong-Heng; Fang, Hong-Hua
  • Advanced Functional Materials, Vol. 28, Issue 35
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Defect Engineering of Grain Boundaries in Lead-Free Halide Double Perovskites for Better Optoelectronic Performance
journal, January 2019

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  • Advanced Functional Materials, Vol. 29, Issue 8
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Tailoring Crystal Structure of FA 0.83 Cs 0.17 PbI 3 Perovskite Through Guanidinium Doping for Enhanced Performance and Tunable Hysteresis of Planar Perovskite Solar Cells
journal, November 2018

  • Pham, Ngoc Duy; Zhang, Chunmei; Tiong, Vincent Tiing
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Charge‐Carrier Dynamics, Mobilities, and Diffusion Lengths of 2D–3D Hybrid Butylammonium–Cesium–Formamidinium Lead Halide Perovskites
journal, June 2019

  • Buizza, Leonardo R. V.; Crothers, Timothy W.; Wang, Zhiping
  • Advanced Functional Materials, Vol. 29, Issue 35
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Thin Insulating Tunneling Contacts for Efficient and Water-Resistant Perovskite Solar Cells
journal, May 2016


From Nanostructural Evolution to Dynamic Interplay of Constituents: Perspectives for Perovskite Solar Cells
journal, March 2018

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Solution Coating of Superior Large-Area Flexible Perovskite Thin Films with Controlled Crystal Packing
journal, May 2017

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  • Advanced Optical Materials, Vol. 5, Issue 11
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Unraveling Photostability of Mixed Cation Perovskite Films in Extreme Environment
journal, August 2018

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  • Advanced Optical Materials, Vol. 6, Issue 20
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Recent Progress in Single-Crystalline Perovskite Research Including Crystal Preparation, Property Evaluation, and Applications
journal, November 2017

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Light-Induced Anomalous Resistive Switches Based on Individual Organic-Inorganic Halide Perovskite Micro-/Nanofibers
journal, July 2018

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Highly Efficient and Stable Perovskite Solar Cells Based on Monolithically Grained CH 3 NH 3 PbI 3 Film
journal, December 2016


Impact of Structural Dynamics on the Optical Properties of Methylammonium Lead Iodide Perovskites
journal, June 2017

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Efficient Passivation with Lead Pyridine‐2‐Carboxylic for High‐Performance and Stable Perovskite Solar Cells
journal, August 2019


Additive Engineering for Efficient and Stable Perovskite Solar Cells
journal, October 2019


Impact of PbI 2 Passivation and Grain Size Engineering in CH 3 NH 3 PbI 3 Solar Absorbers as Revealed by Carrier‐Resolved Photo‐Hall Technique
journal, October 2019

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Emerging Conductive Atomic Force Microscopy for Metal Halide Perovskite Materials and Solar Cells
journal, March 2020

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Perovskite Solar Cells: From the Atomic Level to Film Quality and Device Performance
journal, February 2018

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Scalable Deposition Methods for Large‐area Production of Perovskite Thin Films
journal, June 2019

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The Impact of Nano- and Microstructure on the Stability of Perovskite Solar Cells
journal, October 2018


Visualizing Nonradiative Mobile Defects in Organic–Inorganic Perovskite Materials
journal, April 2019


Short‐Term Stability of Perovskite Solar Cells Affected by In Situ Interface Modification
journal, May 2019


Solar perovskite thin films with enhanced mechanical, thermal, UV, and moisture stability via vacuum-assisted deposition
journal, November 2019

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Stability improvement under high efficiency—next stage development of perovskite solar cells
journal, April 2019


Towards stable and commercially available perovskite solar cells
journal, October 2016


2D perovskite stabilized phase-pure formamidinium perovskite solar cells
journal, August 2018


Microstructural Evolution of Hybrid Perovskites Promoted by Chlorine and its Impact on the Performance of Solar Cell
journal, March 2019


Achieving high-performance thick-film perovskite solar cells with electron transporting Bingel fullerenes
journal, January 2018

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Effect of halide ratio and Cs + addition on the photochemical stability of lead halide perovskites
journal, January 2018

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One-step implementation of plasmon enhancement and solvent annealing effects for air-processed high-efficiency perovskite solar cells
journal, January 2018

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Highly efficient CsPbIBr 2 perovskite solar cells with efficiency over 9.8% fabricated using a preheating-assisted spin-coating method
journal, January 2019

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Ion induced passivation of grain boundaries in perovskite solar cells
journal, May 2019

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Verification and mitigation of ion migration in perovskite solar cells
journal, April 2019

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Identifying inverted-hysteresis behavior of CH 3 NH 3 PbI 3−x Cl x planar hybrid perovskite solar cells based on external bias precondition
journal, July 2019

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Inorganic–organic halide perovskites for new photovoltaic technology
journal, August 2017

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Molecular doping enabled scalable blading of efficient hole-transport-layer-free perovskite solar cells
text, January 2018

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Matching Charge Extraction Contact for Wide-Bandgap Perovskite Solar Cells
text, January 2017

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Unveiling the operation mechanism of layered perovskite solar cells
text, January 2019

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Dopant compensation in alloyed CH3NH3PbBr3-xClx perovskite single crystals for gamma-ray spectroscopy
text, January 2017

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Imperfections and their passivation in halide perovskite solar cells
text, January 2019

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Halide lead perovskites for ionizing radiation detection
text, January 2019

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Understanding charge transport in lead iodide perovskite thin-film field-effect transistors
text, January 2017

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Constructing CsPbBr 3 Cluster Passivated‐Triple Cation Perovskite for Highly Efficient and Operationally Stable Solar Cells
journal, February 2019

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Planar‐Structure Perovskite Solar Cells with Efficiency beyond 21%
journal, October 2017


Imaging Heterogeneously Distributed Photo‐Active Traps in Perovskite Single Crystals
journal, February 2018


Structural and Chemical Changes to CH 3 NH 3 PbI 3 Induced by Electron and Gallium Ion Beams
journal, April 2018


Efficiency and Stability Enhancement of Fully Ambient Air Processed Perovskite Solar Cells Using TiO 2 Paste with Tunable Pore Structure
journal, December 2019

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Efficient and Stable Chemical Passivation on Perovskite Surface via Bidentate Anchoring
journal, February 2019

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Ultrathin Nanosheets of Oxo‐functionalized Graphene Inhibit the Ion Migration in Perovskite Solar Cells
journal, December 2019

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Halide lead perovskites for ionizing radiation detection
journal, March 2019


Colloidal engineering for monolayer CH 3 NH 3 PbI 3 films toward high performance perovskite solar cells
journal, January 2017

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A laminar MAPbBr 3 /MAPbBr 3−x I x graded heterojunction single crystal for enhancing charge extraction and optoelectronic performance
journal, January 2019

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Copper Iodide Interlayer for Improved Charge Extraction and Stability of Inverted Perovskite Solar Cells
journal, April 2019

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Ambient Air Stability of Hybrid Perovskite Thin‐Film Transistors by Ambient Air Processing
journal, January 2020

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Progress in Tandem Solar Cells Based on Hybrid Organic-Inorganic Perovskites
journal, March 2017

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Phase Segregation Enhanced Ion Movement in Efficient Inorganic CsPbIBr 2 Solar Cells
journal, July 2017

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Role of Ionic Functional Groups on Ion Transport at Perovskite Interfaces
journal, August 2017

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Device Physics of Hybrid Perovskite Solar cells: Theory and Experiment
journal, February 2018

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In-situ cross-linking strategy for efficient and operationally stable methylammoniun lead iodide solar cells
journal, September 2018


Surface engineering of perovskite films for efficient solar cells
journal, November 2017


Post-annealing of MAPbI 3 perovskite films with methylamine for efficient perovskite solar cells
journal, January 2016

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Covering effect of conductive glass: a facile route to tailor the grain growth of hybrid perovskites for highly efficient solar cells
journal, January 2018

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Stabilizing halide perovskite surfaces for solar cell operation with wide-bandgap lead oxysalts
text, January 2019

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Giant Zero-Drift Electronic Behaviors in Methylammonium Lead Halide Perovskite Diodes by Doping Iodine Ions
journal, September 2018

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Grain-Boundary “Patches” by In Situ Conversion to Enhance Perovskite Solar Cells Stability
journal, June 2018


Capturing the Sun: A Review of the Challenges and Perspectives of Perovskite Solar Cells
journal, June 2017

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Unveiling the operation mechanism of layered perovskite solar cells
journal, March 2019


Dual‐Phase All‐Inorganic Cesium Halide Perovskites for Conducting‐Bridge Memory‐Based Artificial Synapses
journal, September 2019

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Versatile Defect Passivation Methods for Metal Halide Perovskite Materials and their Application to Light‐Emitting Devices
journal, December 2018


Additional Organic‐Solvent‐Rinsing Process to Enhance Perovskite Photovoltaic Performance
journal, July 2019

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Efficient Semitransparent Perovskite Solar Cells for 23.0%-Efficiency Perovskite/Silicon Four-Terminal Tandem Cells
journal, July 2016


Evolution of Photovoltaic Performance in Fully Printable Mesoscopic Carbon‐Based Perovskite Solar Cells
journal, May 2019


Trifluoroacetate induced small-grained CsPbBr3 perovskite films result in efficient and stable light-emitting devices
journal, February 2019


Large lattice distortions and size-dependent bandgap modulation in epitaxial halide perovskite nanowires
journal, January 2020


Electrochemical and atomic force microscopy investigations of the effect of CdS on the local electrical properties of CH 3 NH 3 PbI 3 :CdS perovskite solar cells
journal, January 2017

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Perspective: Theory and simulation of hybrid halide perovskites
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Ion Induced Passivation of Grain Boundaries in Perovskite Solar Cells
text, January 2018