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Title: Dipolar cations confer defect tolerance in wide-bandgap metal halide perovskites

Journal Article · · Nature Communications
 [1];  [2];  [2];  [2];  [2];  [2];  [3];  [2];  [4];  [2]; ORCiD logo [2];  [2]; ORCiD logo [5];  [6];  [2]; ORCiD logo [2]; ORCiD logo [2];  [3]; ORCiD logo [2]
  1. Univ. of Toronto, ON (Canada). Dept. of Electrical and Computer Engineering; Nanjing Univ. (China). National Lab. of Solid State Microstructures. Collaborative Innovation Centre of Advanced Microstructures. Jiangsu Key Lab. of Artificial Functional Materials. College of Engineering and Applied Sciences
  2. Univ. of Toronto, ON (Canada). Dept. of Electrical and Computer Engineering
  3. Univ. of California, Berkeley, CA (United States). Dept. of Materials Science and Engineering; Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States). Materials Sciences Division
  4. Univ. of Toronto, ON (Canada). Dept. of Electrical and Computer Engineering; Henan Univ., Kaifeng (China). Key Lab. of Photovoltaic Materials. Dept. of Physics and Electronics
  5. Univ. of Toronto, ON (Canada). Dept. of Electrical and Computer Engineering; KU Leuven (Belgium). Dept. of Chemistry
  6. KU Leuven (Belgium). Dept. of Chemistry

Efficient wide-bandgap perovskite solar cells (PSCs) enable high-efficiency tandem photovoltaics when combined with crystalline silicon and other low-bandgap absorbers. However, wide-bandgap PSCs today exhibit performance far inferior to that of sub-1.6-eV bandgap PSCs due to their tendency to form a high density of deep traps. Here, we show that healing the deep traps in wide-bandgap perovskites—in effect, increasing the defect tolerance via cation engineering—enables further performance improvements in PSCs. We achieve a stabilized power conversion efficiency of 20.7% for 1.65-eV bandgap PSCs by incorporating dipolar cations, with a high open-circuit voltage of 1.22 V and a fill factor exceeding 80%. We also obtain a stabilized efficiency of 19.1% for 1.74-eV bandgap PSCs with a high open-circuit voltage of 1.25 V. From density functional theory calculations, we find that the presence and reorientation of the dipolar cation in mixed cation–halide perovskites heals the defects that introduce deep trap states.

Research Organization:
Lawrence Berkeley National Laboratory (LBNL), Berkeley, CA (United States)
Sponsoring Organization:
USDOE Office of Science (SC), Basic Energy Sciences (BES); Office of Naval Research (ONR) (United States); King Abdullah Univ. of Science and Technology (KAUST) (Saudi Arabia); Ontario Research Fund Research Excellence Program (Canada); Natural Sciences and Engineering Research Council of Canada (NSERC); Netherlands Organisation for Scientific Research (NWO); Thousand Talent Program for Young Outstanding Scientists (China)
Grant/Contract Number:
AC02-05CH11231; N00014-17-1-2524; OSR-2017-CPF-3321-03; 680-50-1511
OSTI ID:
1477412
Journal Information:
Nature Communications, Vol. 9; ISSN 2041-1723
Publisher:
Nature Publishing GroupCopyright Statement
Country of Publication:
United States
Language:
English
Citation Metrics:
Cited by: 216 works
Citation information provided by
Web of Science

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Synergistic Effects of Lead Thiocyanate Additive and Solvent Annealing on the Performance of Wide-Bandgap Perovskite Solar Cells journal April 2017
Modeling the Performance Limitations and Prospects of Perovskite/Si Tandem Solar Cells under Realistic Operating Conditions journal August 2017
The Potential of Multijunction Perovskite Solar Cells journal October 2017
Universal Dynamics of Molecular Reorientation in Hybrid Lead Iodide Perovskites journal November 2017
Materials Processing Routes to Trap-Free Halide Perovskites journal October 2014
Compositional engineering of perovskite materials for high-performance solar cells journal January 2015
Photo-induced halide redistribution in organic–inorganic perovskite films journal May 2016
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Polar rotor scattering as atomic-level origin of low mobility and thermal conductivity of perovskite CH3NH3PbI3 journal June 2017
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The dynamics of methylammonium ions in hybrid organic–inorganic perovskite solar cells journal May 2015
Correlation of energy disorder and open-circuit voltage in hybrid perovskite solar cells journal January 2016
Hybrid perovskite films approaching the radiative limit with over 90% photoluminescence quantum efficiency journal April 2018
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Determination of defect distributions from admittance measurements and application to Cu(In,Ga)Se 2 based heterojunctions journal October 1996
A mixed-cation lead mixed-halide perovskite absorber for tandem solar cells journal January 2016
Screening in crystalline liquids protects energetic carriers in hybrid perovskites journal September 2016
Incorporation of rubidium cations into perovskite solar cells improves photovoltaic performance journal September 2016
Efficient and stable solution-processed planar perovskite solar cells via contact passivation journal February 2017
Long-range hot-carrier transport in hybrid perovskites visualized by ultrafast microscopy journal April 2017
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Accelerating the Screening of Perovskite Compositions for Photovoltaic Applications through High‐Throughput Inkjet Printing journal October 2019
Design of an Inorganic Mesoporous Hole‐Transporting Layer for Highly Efficient and Stable Inverted Perovskite Solar Cells journal November 2018
Semitransparent Perovskite Solar Cells: From Materials and Devices to Applications journal August 2019
Defect and Contact Passivation for Perovskite Solar Cells journal April 2019
A‐Site Management for Highly Crystalline Perovskites journal November 2019
Cesium Lead Inorganic Solar Cell with Efficiency beyond 18% via Reduced Charge Recombination journal October 2019
Combining Efficiency and Stability in Mixed Tin–Lead Perovskite Solar Cells by Capping Grains with an Ultrathin 2D Layer journal March 2020
One‐Step Loading on Natural Mineral Halloysite Nanotube: An Effective Way to Enhance the Stability of Perovskite CsPbX 3 (X = Cl, Br, I) Quantum Dots journal December 2018
Reducing Saturation-Current Density to Realize High-Efficiency Low-Bandgap Mixed Tin-Lead Halide Perovskite Solar Cells journal November 2018
Progress of Surface Science Studies on ABX 3 ‐Based Metal Halide Perovskite Solar Cells journal April 2020
Wide‐Bandgap Perovskite/Gallium Arsenide Tandem Solar Cells journal December 2019
New Strategies for Defect Passivation in High‐Efficiency Perovskite Solar Cells journal April 2020
Verringerung schädlicher Defekte für leistungsstarke Metallhalogenid‐Perowskit‐Solarzellen journal April 2020
Enhanced Lifetime and Photostability with Low‐Temperature Mesoporous ZnTiO 3 /Compact SnO 2 Electrodes in Perovskite Solar Cells journal November 2019
Reducing Detrimental Defects for High‐Performance Metal Halide Perovskite Solar Cells journal January 2020
Two‐Terminal Perovskites Tandem Solar Cells: Recent Advances and Perspectives journal May 2019
Light Management in Monolithic Perovskite/Silicon Tandem Solar Cells journal August 2019
Revealing the crystallization process and realizing uniform 1.8 eV MA-based wide-bandgap mixed-halide perovskites via solution engineering journal February 2019
Binary organic spacer-based quasi-two-dimensional perovskites with preferable vertical orientation and efficient charge transport for high-performance planar solar cells journal January 2019
Progress in air-processed perovskite solar cells: from crystallization to photovoltaic performance journal January 2019
LEDs using halide perovskite nanocrystal emitters journal January 2019
On understanding bandgap bowing and optoelectronic quality in Pb–Sn alloy hybrid perovskites journal January 2019
Molecular modulator for stable inverted planar perovskite solar cells with efficiency enhanced by interface engineering journal January 2019
Wide-bandgap, low-bandgap, and tandem perovskite solar cells journal July 2019
Understanding macroscale functionality of metal halide perovskites in terms of nanoscale heterogeneities journal December 2018
Cesium Lead Inorganic Solar Cell with Efficiency beyond 18% via Reduced Charge Recombination journal March 2021
Enhanced Lifetime and Photostability with Low‐Temperature Mesoporous ZnTiO 3 /Compact SnO 2 Electrodes in Perovskite Solar Cells journal November 2019
New Strategies for Defect Passivation in High-Efficiency Perovskite Solar Cells text January 2020
Monitoring Charge Carrier Diffusion across a Perovskite Film with Transient Absorption Spectroscopy journal December 2019