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Title: Non-wetting surface-driven high-aspect-ratio crystalline grain growth for efficient hybrid perovskite solar cells

Abstract

Large-aspect-ratio grains are needed in polycrystalline thin-film solar cells for reduced charge recombination at grain boundaries; however, the grain size in organolead trihalide perovskite (OTP) films is generally limited by the film thickness. Here we report the growth of OTP grains with high average aspect ratio of 2.3–7.9 on a wide range of non-wetting hole transport layers (HTLs), which increase nucleus spacing by suppressing heterogeneous nucleation and facilitate grain boundary migration in grain growth by imposing less drag force. The reduced grain boundary area and improved crystallinity dramatically reduce the charge recombination in OTP thin films to the level in OTP single crystals. Combining the high work function of several HTLs, a high stabilized device efficiency of 18.3% in low-temperature-processed planar-heterojunction OTP devices under 1 sun illumination is achieved. As a result, this simple method in enhancing OTP morphology paves the way for its application in other optoelectronic devices for enhanced performance.

Authors:
 [1];  [1];  [1];  [1];  [1];  [1]
  1. Univ. of Nebraska, Lincoln, NE (United States)
Publication Date:
Research Org.:
Univ. of Nebraska, Lincoln, NE (United States)
Sponsoring Org.:
USDOE
OSTI Identifier:
1238043
Grant/Contract Number:  
EE0006709
Resource Type:
Accepted Manuscript
Journal Name:
Nature Communications
Additional Journal Information:
Journal Volume: 6; Journal Issue: 2; Journal ID: ISSN 2041-1723
Publisher:
Nature Publishing Group
Country of Publication:
United States
Language:
English
Subject:
36 MATERIALS SCIENCE; physical sciences; applied physics; materials science

Citation Formats

Bi, Cheng, Wang, Qi, Shao, Yuchuan, Yuan, Yongbo, Xiao, Zhengguo, and Huang, Jinsong. Non-wetting surface-driven high-aspect-ratio crystalline grain growth for efficient hybrid perovskite solar cells. United States: N. p., 2015. Web. doi:10.1038/ncomms8747.
Bi, Cheng, Wang, Qi, Shao, Yuchuan, Yuan, Yongbo, Xiao, Zhengguo, & Huang, Jinsong. Non-wetting surface-driven high-aspect-ratio crystalline grain growth for efficient hybrid perovskite solar cells. United States. https://doi.org/10.1038/ncomms8747
Bi, Cheng, Wang, Qi, Shao, Yuchuan, Yuan, Yongbo, Xiao, Zhengguo, and Huang, Jinsong. Mon . "Non-wetting surface-driven high-aspect-ratio crystalline grain growth for efficient hybrid perovskite solar cells". United States. https://doi.org/10.1038/ncomms8747. https://www.osti.gov/servlets/purl/1238043.
@article{osti_1238043,
title = {Non-wetting surface-driven high-aspect-ratio crystalline grain growth for efficient hybrid perovskite solar cells},
author = {Bi, Cheng and Wang, Qi and Shao, Yuchuan and Yuan, Yongbo and Xiao, Zhengguo and Huang, Jinsong},
abstractNote = {Large-aspect-ratio grains are needed in polycrystalline thin-film solar cells for reduced charge recombination at grain boundaries; however, the grain size in organolead trihalide perovskite (OTP) films is generally limited by the film thickness. Here we report the growth of OTP grains with high average aspect ratio of 2.3–7.9 on a wide range of non-wetting hole transport layers (HTLs), which increase nucleus spacing by suppressing heterogeneous nucleation and facilitate grain boundary migration in grain growth by imposing less drag force. The reduced grain boundary area and improved crystallinity dramatically reduce the charge recombination in OTP thin films to the level in OTP single crystals. Combining the high work function of several HTLs, a high stabilized device efficiency of 18.3% in low-temperature-processed planar-heterojunction OTP devices under 1 sun illumination is achieved. As a result, this simple method in enhancing OTP morphology paves the way for its application in other optoelectronic devices for enhanced performance.},
doi = {10.1038/ncomms8747},
journal = {Nature Communications},
number = 2,
volume = 6,
place = {United States},
year = {Mon Jul 20 00:00:00 EDT 2015},
month = {Mon Jul 20 00:00:00 EDT 2015}
}

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journal, February 2019

  • Liu, Yuqiang; Wu, Tian; Liu, Yuan
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Ion induced passivation of grain boundaries in perovskite solar cells
journal, May 2019

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Towards large-area perovskite solar cells: the influence of compact and mesoporous TiO 2 electron transport layers
journal, July 2018


The roles of acetylacetone additives in enhancing perovskite solar cell performance
journal, November 2018


The effect of substrate temperature on microstructural evolution and hardenability of tungsten carbide coating in hot filament chemical vapor deposition
journal, April 2018

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Ultrahigh sensitivity of methylammonium lead tribromide perovskite single crystals to environmental gases
journal, July 2016

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Integrating Ultrathin Bulk-Heterojunction Organic Semiconductor Intermediary for High-Performance Low-Bandgap Perovskite Solar Cells with Low Energy Loss
journal, August 2018

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Low‐Bandgap Mixed Tin‐Lead Perovskites and Their Applications in All‐Perovskite Tandem Solar Cells
journal, February 2019

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“Liquid Knife” to Fabricate Patterning Single-Crystalline Perovskite Microplates toward High-Performance Laser Arrays
journal, March 2016


Employing Lead Thiocyanate Additive to Reduce the Hysteresis and Boost the Fill Factor of Planar Perovskite Solar Cells
journal, May 2016

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A Review on Organic-Inorganic Halide Perovskite Photodetectors: Device Engineering and Fundamental Physics
journal, September 2017


Efficient Flexible Solar Cell based on Composition-Tailored Hybrid Perovskite
journal, June 2017


The Electrical and Optical Properties of Organometal Halide Perovskites Relevant to Optoelectronic Performance
journal, October 2017

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Critical Role of Interface and Crystallinity on the Performance and Photostability of Perovskite Solar Cell on Nickel Oxide
journal, December 2017

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

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Stable High-Performance Perovskite Solar Cells via Grain Boundary Passivation
journal, March 2018


Toward Perovskite Solar Cell Commercialization: A Perspective and Research Roadmap Based on Interfacial Engineering
journal, June 2018

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Dopant‐Free Small‐Molecule Hole‐Transporting Material for Inverted Perovskite Solar Cells with Efficiency Exceeding 21%
journal, July 2019


Modulate Molecular Interaction between Hole Extraction Polymers and Lead Ions toward Hysteresis-Free and Efficient Perovskite Solar Cells
journal, June 2018

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Atomic Layer Deposited TiO 2 -IrO x Alloy as a Hole Transport Material for Perovskite Solar Cells
journal, July 2018

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Stabilized Wide Bandgap MAPbBr x I 3- x Perovskite by Enhanced Grain Size and Improved Crystallinity
journal, December 2015


Recent Progress on the Long-Term Stability of Perovskite Solar Cells
journal, February 2018


Fullerene-Based Materials for Photovoltaic Applications: Toward Efficient, Hysteresis-Free, and Stable Perovskite Solar Cells
journal, December 2017

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

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Efficient and Hysteresis-Free Perovskite Solar Cells Based on a Solution Processable Polar Fullerene Electron Transport Layer
journal, August 2017

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Applications of Phosphorene and Black Phosphorus in Energy Conversion and Storage Devices
journal, December 2017

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Low-Temperature Solution-Processed CuCrO 2 Hole-Transporting Layer for Efficient and Photostable Perovskite Solar Cells
journal, January 2018

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Simultaneous Improvement in Efficiency and Stability of Low-Temperature-Processed Perovskite Solar Cells by Interfacial Control
journal, January 2018

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High-Performance Thickness Insensitive Perovskite Solar Cells with Enhanced Moisture Stability
journal, June 2018

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Simple, Robust, and Going More Efficient: Recent Advance on Electron Transport Layer‐Free Perovskite Solar Cells
journal, May 2019


New Strategies for Defect Passivation in High‐Efficiency Perovskite Solar Cells
journal, April 2020

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Soft Template‐Controlled Growth of High‐Quality CsPbI 3 Films for Efficient and Stable Solar Cells
journal, January 2020


Dithiafulvenyl-Naphthalenediimide-based Small Molecules as efficient Non-Fullerene Electron-Transport Layer for Inverted Perovskite Solar Cells
journal, August 2018

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Advances in Inkjet‐Printed Metal Halide Perovskite Photovoltaic and Optoelectronic Devices
journal, April 2020

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Triphenylamine dibenzofulvene–derived dopant‐free hole transporting layer induces micrometer‐sized perovskite grains for highly efficient near 20% for p‐i‐n perovskite solar cells
journal, October 2019

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Environmental-Friendly Urea Additive Induced Large Perovskite Grains for High Performance Inverted Solar Cells
journal, April 2018


From Macroscopic to Nanoscopic Current Hysteresis Suppressed by Fullerene in Perovskite Solar Cells
journal, August 2019


Effects of precursor composition on morphology and microstructure of hybrid organic–inorganic perovskite solar cells
journal, June 2019


Green light-emitting diodes based on hybrid perovskite films with mixed cesium and methylammonium cations
journal, February 2017


Correlation of energy disorder and open-circuit voltage in hybrid perovskite solar cells
journal, January 2016


Sensitive X-ray detectors made of methylammonium lead tribromide perovskite single crystals
journal, March 2016


Perovskite seeding growth of formamidinium-lead-iodide-based perovskites for efficient and stable solar cells
journal, April 2018


Growth, characterization, and thin film transistor application of CH 3 NH 3 PbI 3 perovskite on polymeric gate dielectric layers
journal, January 2017

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ITIC surface modification to achieve synergistic electron transport layer enhancement for planar-type perovskite solar cells with efficiency exceeding 20%
journal, January 2017

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High mobility, hole transport materials for highly efficient PEDOT:PSS replacement in inverted perovskite solar cells
journal, January 2017

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Degradation of encapsulated perovskite solar cells driven by deep trap states and interfacial deterioration
journal, January 2018

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Improved performance and stability of perovskite solar cells with bilayer electron-transporting layers
journal, January 2018


Critical roles of potassium in charge-carrier balance and diffusion induced defect passivation for efficient inverted perovskite solar cells
journal, January 2019

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Nickel phthalocyanine as an excellent hole-transport material in inverted planar perovskite solar cells
journal, January 2019

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Engineering the underlying surface to manipulate the growth of 2D perovskites for highly efficient solar cells
journal, January 2019

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Control of aggregation and dissolution of small molecule hole transport layers via a doping strategy for highly efficient perovskite solar cells
journal, January 2019

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Functional graded fullerene derivatives for improving the fill factor and device stability of inverted-type perovskite solar cells
journal, May 2018


High-performance perovskite/Cu(In,Ga)Se 2 monolithic tandem solar cells
journal, August 2018


Stable Perovskite Solar Cells with Improved Hydrophobicity Based on BHT Additive
journal, February 2019


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

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Efficient and Stable Perovskite Solar Cells via Dual Functionalization of Dopamine Semiquinone Radical with Improved Trap Passivation Capabilities
journal, March 2018

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Synergistic Coassembly of Highly Wettable and Uniform Hole‐Extraction Monolayers for Scaling‐up Perovskite Solar Cells
journal, December 2019

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NiO x Electrode Interlayer and CH 3 NH 2 /CH 3 NH 3 PbBr 3 Interface Treatment to Markedly Advance Hybrid Perovskite-Based Light-Emitting Diodes
journal, August 2016

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Fully Solution-Processed n-i-p-Like Perovskite Solar Cells with Planar Junction: How the Charge Extracting Layer Determines the Open-Circuit Voltage
journal, January 2017

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MXene‐Derived Ferroelectric Crystals
journal, February 2019


The Role of the Interfaces in Perovskite Solar Cells
journal, November 2019

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Improving Interfacial Charge Recombination in Planar Heterojunction Perovskite Photovoltaics with Small Molecule as Electron Transport Layer
journal, May 2017

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Strategic Synthesis of Ultrasmall NiCo 2 O 4 NPs as Hole Transport Layer for Highly Efficient Perovskite Solar Cells
journal, February 2018


The Role of Charge Selective Contacts in Perovskite Solar Cell Stability
journal, December 2018


Efficient and Stable Inverted Planar Perovskite Solar Cells Using a Triphenylamine Hole-Transporting Material
journal, April 2018


A Cytop Insulating Tunneling Layer for Efficient Perovskite Solar Cells
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One‐Step Inkjet Printed Perovskite in Air for Efficient Light Harvesting
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Enhancing the performance of perovskite solar cells via interface modification
journal, August 2019


Hybrid organic—inorganic perovskites: low-cost semiconductors with intriguing charge-transport properties
journal, January 2016

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Polymer-templated nucleation and crystal growth of perovskite films for solar cells with efficiency greater than 21%
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Ultra-high open-circuit voltage of perovskite solar cells induced by nucleation thermodynamics on rough substrates
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Improved power conversion efficiency of perovskite solar cells using highly conductive WO x doped PEDOT:PSS
journal, January 2018

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Highly efficient inverted perovskite solar cells based on self-assembled graphene derivatives
journal, January 2018

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Incorporating deep electron traps into perovskite devices: towards high efficiency solar cells and fast photodetectors
journal, January 2018

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Bi-functional additive engineering for high-performance perovskite solar cells with reduced trap density
journal, January 2019

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Low temperature and rapid formation of high quality metal oxide thin film via a hydroxide-assisted energy conservation strategy
journal, January 2018

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Hierarchy of interfacial passivation in inverted perovskite solar cells
journal, January 2019

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Overcoming intrinsic defects of the hole transport layer with optimized carbon nanorods for perovskite solar cells
journal, January 2019

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Sulfur-fused perylene diimide electron transport layers allow >400 h operational lifetime of methylammonium lead iodide photovoltaics
journal, January 2019

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The effect of hole transporting layer in charge accumulation properties of p-i-n perovskite solar cells
journal, July 2017

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Mixed Halide Perovskite Solar Cells: Progress and Challenges
journal, February 2019

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Formation and characterization of preferred oriented perovskite thin films on single-crystalline substrates
journal, June 2018

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Enhanced photovoltage for inverted planar heterojunction perovskite solar cells
journal, June 2018


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

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Argon Plasma Treatment to Tune Perovskite Surface Composition for High Efficiency Solar Cells and Fast Photodetectors
text, January 2018

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All-Inorganic Perovskite Solar Cells Based on CsPbIBr2 and Metal Oxide Transport Layers with Improved Stability
journal, November 2019

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Achieving 20% Efficiency for Low‐Temperature‐Processed Inverted Perovskite Solar Cells
journal, December 2018

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Defect and Contact Passivation for Perovskite Solar Cells
journal, April 2019

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Advances in Perovskite Solar Cells
journal, January 2016


Light-Induced Self-Poling Effect on Organometal Trihalide Perovskite Solar Cells for Increased Device Efficiency and Stability
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Interfaces in Perovskite Solar Cells
journal, August 2017

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A Lewis Base-Assisted Passivation Strategy Towards Highly Efficient and Stable Perovskite Solar Cells
journal, May 2018


Interfacial Post‐Treatment for Enhancing the Performance of Printable Carbon‐Based Perovskite Solar Cells
journal, July 2019


Spiro‐Linked Molecular Hole‐Transport Materials for Highly Efficient Inverted Perovskite Solar Cells
journal, November 2019


Electron Transporting Bilayer of SnO 2 and TiO 2 Nanocolloid Enables Highly Efficient Planar Perovskite Solar Cells
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Investigation into the Advantages of Pure Perovskite Film without PbI2 for High Performance Solar Cell
journal, October 2016

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Air-stable formamidinium/methylammonium mixed lead iodide perovskite integral microcrystals with low trap density and high photo-responsivity
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Efficient and UV-stable perovskite solar cells enabled by side chain-engineered polymeric hole-transporting layers
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Meniscus fabrication of halide perovskite thin films at high throughput for large area and low-cost solar panels
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Quantification of re-Absorption and re-emission processes to determine photon recycling efficiency in perovskite single crystals
text, January 2017

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Enhancing stability and efficiency of perovskite solar cells with crosslinkable silane-functionalized and doped fullerene
text, January 2016

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Crystallization kinetics and morphology control of formamidinium-cesium mixed-cation lead mixed-halide perovskite via tunability of the colloidal precursor solution
conference, January 2018


Improving Two-Step Prepared CH3NH3PbI3 Perovskite Solar Cells by Co-Doping Potassium Halide and Water in PbI2 Layer
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Acidity Suppression of Hole Transport Layer via Solution Reaction of Neutral PEDOT:PSS for Stable Perovskite Photovoltaics
journal, January 2020


Growth modes and quantum confinement in ultrathin vapour-deposited MAPbI₃ films
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Conjugated Small Molecule for Efficient Hole Transport in High-Performance p-i-n Type Perovskite Solar Cells
journal, July 2017

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Solution‐Processable Perovskite Solar Cells toward Commercialization: Progress and Challenges
journal, April 2019

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Double‐Sided Surface Passivation of 3D Perovskite Film for High‐Efficiency Mixed‐Dimensional Perovskite Solar Cells
journal, December 2019

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Achieving Large-Area Planar Perovskite Solar Cells by Introducing an Interfacial Compatibilizer
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Cost-Performance Analysis of Perovskite Solar Modules
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Air-Stable, Efficient Mixed-Cation Perovskite Solar Cells with Cu Electrode by Scalable Fabrication of Active Layer
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How does alkyl chain length modify the properties of triphenylamine-based hole transport materials?
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A Cu 3 PS 4 nanoparticle hole selective layer for efficient inverted perovskite solar cells
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Electronic transport of organic-inorganic hybrid perovskites from first-principles and machine learning
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Improved Efficiency and Stability of Perovskite Solar Cells Induced by CO Functionalized Hydrophobic Ammonium‐Based Additives
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Engineering of the Back Contact between PCBM and Metal Electrode for Planar Perovskite Solar Cells with Enhanced Efficiency and Stability
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SrTiO 3 /Al 2 O 3 ‐Graphene Electron Transport Layer for Highly Stable and Efficient Composites‐Based Perovskite Solar Cells with 20.6% Efficiency
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Co‐Electrodeposition of Sn‐Doped TiO 2 Electron‐Transporting Layer for Perovskite Solar Cells
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Bifacial Contact Junction Engineering for High‐Performance Perovskite Solar Cells with Efficiency Exceeding 21%
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Polyfluorene Copolymers as High‐Performance Hole‐Transport Materials for Inverted Perovskite Solar Cells
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Unveiling the synergistic effect of precursor stoichiometry and interfacial reactions for perovskite light-emitting diodes
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Ultrasmooth metal halide perovskite thin films via sol–gel processing
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Improving the photovoltaic performance of planar heterojunction perovskite solar cells by mixed solvent vapor treatment
journal, January 2018

  • Yuan, Binbin; Zhao, Suling; Xu, Zheng
  • RSC Advances, Vol. 8, Issue 21
  • DOI: 10.1039/c7ra13289a

The Effect of Hole Transporting Layer in Charge Accumulation Properties of p-i-n Perovskite Solar Cells
text, January 2018


Stabilized Wide Bandgap MAPbBr x I 3- x Perovskite by Enhanced Grain Size and Improved Crystallinity
journal, December 2015


Advances in Perovskite Solar Cells
journal, January 2016


Recent Progress on the Long-Term Stability of Perovskite Solar Cells
journal, February 2018


Aqueous-Containing Precursor Solutions for Efficient Perovskite Solar Cells
journal, November 2017

  • Liu, Dianyi; Traverse, Christopher J.; Chen, Pei
  • Advanced Science, Vol. 5, Issue 1
  • DOI: 10.1002/advs.201700484

Recent Advance in Solution-Processed Organic Interlayers for High-Performance Planar Perovskite Solar Cells
journal, May 2018

  • Zhang, Wenxiao; Wang, Ying-Chiao; Li, Xiaodong
  • Advanced Science, Vol. 5, Issue 7
  • DOI: 10.1002/advs.201800159

Ultrathin Hole Extraction Layer for Efficient Inverted Perovskite Solar Cells
journal, June 2018


Optimizing Lignosulfonic Acid-Grafted Polyaniline as a Hole-Transport Layer for Inverted CH3NH3PbI3 Perovskite Solar Cells
journal, January 2020


Thin single crystal perovskite solar cells to harvest below-bandgap light absorption
journal, December 2017


Perovskite seeding growth of formamidinium-lead-iodide-based perovskites for efficient and stable solar cells
journal, April 2018


Publisher Correction: All-inorganic cesium lead iodide perovskite solar cells with stabilized efficiency beyond 15%
journal, November 2018


Tailoring vertical phase distribution of quasi-two-dimensional perovskite films via surface modification of hole-transporting layer
journal, February 2019


Structural and Photophysical Properties of Methylammonium Lead Tribromide (MAPbBr3) Single Crystals
journal, October 2017


Scalable ultrafast epitaxy of large-grain and single-crystal II-VI semiconductors
journal, February 2020


Ti/Au Cathode for Electronic transport material-free organic-inorganic hybrid perovskite solar cells
journal, December 2016

  • Shi, Tongfei; Chen, Jian; Zheng, Jianqiang
  • Scientific Reports, Vol. 6, Issue 1
  • DOI: 10.1038/srep39132

Ultrahigh sensitivity of methylammonium lead tribromide perovskite single crystals to environmental gases
journal, July 2016

  • Fang, Hong-Hua; Adjokatse, Sampson; Wei, Haotong
  • Science Advances, Vol. 2, Issue 7
  • DOI: 10.1126/sciadv.1600534

Effects of Aromatic Ammoniums on Methyl Ammonium Lead Iodide Hybrid Perovskite Materials
journal, January 2017


Excess charge-carrier induced instability of hybrid perovskites
text, January 2018

  • Y., Fang,; B., Chen,; Y., Lin,
  • The University of North Carolina at Chapel Hill University Libraries
  • DOI: 10.17615/qj2r-3306

Overcoming the Intrinsic Difference between Hydrophilic CH3NH3PbI3 and Hydrophobic C60 Thin Films to Improve the Photovoltaic Performance
journal, July 2017

  • Chen, Lung-Chien; Lin, Yu-Shiang; Tseng, Zong-Liang
  • Nanomaterials, Vol. 7, Issue 7
  • DOI: 10.3390/nano7070166

Improved Efficiency of Perovskite Solar Cells by the Interfacial Modification of the Active Layer
journal, February 2019

  • Lu, Zhen; Wang, Shangzhi; Liu, Huijun
  • Nanomaterials, Vol. 9, Issue 2
  • DOI: 10.3390/nano9020204

All-Inorganic Perovskite Solar Cells Based on CsPbIBr2 and Metal Oxide Transport Layers with Improved Stability
journal, November 2019

  • Yang, Jien; Zhang, Qiong; Xu, Jinjin
  • Nanomaterials, Vol. 9, Issue 12
  • DOI: 10.3390/nano9121666