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Title: Perovskite Solar Cells with Near 100% Internal Quantum Efficiency Based on Large Single Crystalline Grains and Vertical Bulk Heterojunctions

Abstract

Grain boundaries (GBs) as defects in the crystal lattice detrimentally impact the power conversion efficiency (PCE) of polycrystalline solar cells, particularly in recently emerging hybrid perovskites where non-radiative recombination processes lead to significant carrier losses. Here, the beneficial effects of activated vertical GBs are demonstrated by first growing large, vertically-oriented methylammonium lead tri-iodide (CH3NH3PbI3) single-crystalline grains. We show that infiltration of p-type doped 2 -7,7 -tetrakis(N,Ndi-p-methoxyphenylamine)-9,9-spirobifluorene (Spiro-OMeTAD) into CH3NH3PbI3 films along the GBs creates space charge regions to suppress non-radiative recombination and enhance carrier collection efficiency. Solar cells with such activated GBs yielded average PCE of 16.3 ± 0.9%, which are among the best solution-processed perovskite devices. As an important alternative to growing ideal CH3NH3PbI3 single crystal films, which is difficult to achieve for such fast-crystallizing perovskites, activating GBs paves a way to design a new type of bulk heterojunction hybrid perovskite photovoltaics toward theoretical maximum PCE.

Authors:
 [1];  [2];  [1];  [1];  [1];  [2];  [1];  [1];  [2];  [1];  [1]
  1. Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States)
  2. Univ. of Tennessee, Knoxville, TN (United States)
Publication Date:
Research Org.:
Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States). Center for Nanophase Materials Sciences (CNMS)
Sponsoring Org.:
USDOE Office of Science (SC)
OSTI Identifier:
1209201
Grant/Contract Number:  
AC05-00OR22725
Resource Type:
Journal Article: Accepted Manuscript
Journal Name:
Journal of the American Chemical Society
Additional Journal Information:
Journal Volume: 137; Journal Issue: 29; Journal ID: ISSN 0002-7863
Publisher:
American Chemical Society (ACS)
Country of Publication:
United States
Language:
English
Subject:
14 SOLAR ENERGY

Citation Formats

Yang, Bin, Dyck, Ondrej, Poplawsky, Jonathan, Keum, Jong, Puretzky, Alexander, Das, Sanjib, Ivanov, Ilia, Rouleau, Christopher, Duscher, Gerd, Geohegan, David, and Xiao, Kai. Perovskite Solar Cells with Near 100% Internal Quantum Efficiency Based on Large Single Crystalline Grains and Vertical Bulk Heterojunctions. United States: N. p., 2015. Web. doi:10.1021/jacs.5b03144.
Yang, Bin, Dyck, Ondrej, Poplawsky, Jonathan, Keum, Jong, Puretzky, Alexander, Das, Sanjib, Ivanov, Ilia, Rouleau, Christopher, Duscher, Gerd, Geohegan, David, & Xiao, Kai. Perovskite Solar Cells with Near 100% Internal Quantum Efficiency Based on Large Single Crystalline Grains and Vertical Bulk Heterojunctions. United States. https://doi.org/10.1021/jacs.5b03144
Yang, Bin, Dyck, Ondrej, Poplawsky, Jonathan, Keum, Jong, Puretzky, Alexander, Das, Sanjib, Ivanov, Ilia, Rouleau, Christopher, Duscher, Gerd, Geohegan, David, and Xiao, Kai. 2015. "Perovskite Solar Cells with Near 100% Internal Quantum Efficiency Based on Large Single Crystalline Grains and Vertical Bulk Heterojunctions". United States. https://doi.org/10.1021/jacs.5b03144. https://www.osti.gov/servlets/purl/1209201.
@article{osti_1209201,
title = {Perovskite Solar Cells with Near 100% Internal Quantum Efficiency Based on Large Single Crystalline Grains and Vertical Bulk Heterojunctions},
author = {Yang, Bin and Dyck, Ondrej and Poplawsky, Jonathan and Keum, Jong and Puretzky, Alexander and Das, Sanjib and Ivanov, Ilia and Rouleau, Christopher and Duscher, Gerd and Geohegan, David and Xiao, Kai},
abstractNote = {Grain boundaries (GBs) as defects in the crystal lattice detrimentally impact the power conversion efficiency (PCE) of polycrystalline solar cells, particularly in recently emerging hybrid perovskites where non-radiative recombination processes lead to significant carrier losses. Here, the beneficial effects of activated vertical GBs are demonstrated by first growing large, vertically-oriented methylammonium lead tri-iodide (CH3NH3PbI3) single-crystalline grains. We show that infiltration of p-type doped 2 -7,7 -tetrakis(N,Ndi-p-methoxyphenylamine)-9,9-spirobifluorene (Spiro-OMeTAD) into CH3NH3PbI3 films along the GBs creates space charge regions to suppress non-radiative recombination and enhance carrier collection efficiency. Solar cells with such activated GBs yielded average PCE of 16.3 ± 0.9%, which are among the best solution-processed perovskite devices. As an important alternative to growing ideal CH3NH3PbI3 single crystal films, which is difficult to achieve for such fast-crystallizing perovskites, activating GBs paves a way to design a new type of bulk heterojunction hybrid perovskite photovoltaics toward theoretical maximum PCE.},
doi = {10.1021/jacs.5b03144},
url = {https://www.osti.gov/biblio/1209201}, journal = {Journal of the American Chemical Society},
issn = {0002-7863},
number = 29,
volume = 137,
place = {United States},
year = {2015},
month = {7}
}

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Works referenced in this record:

Efficient planar heterojunction perovskite solar cells by vapour deposition
journal, September 2013


Electron-hole diffusion lengths > 175 μm in solution-grown CH 3 NH 3 PbI 3 single crystals
journal, January 2015


Lead-free solid-state organic–inorganic halide perovskite solar cells
journal, May 2014


Sequential deposition as a route to high-performance perovskite-sensitized solar cells
journal, July 2013


Solvent engineering for high-performance inorganic–organic hybrid perovskite solar cells
journal, July 2014


Organometal Halide Perovskites as Visible-Light Sensitizers for Photovoltaic Cells
journal, May 2009


6.5% efficient perovskite quantum-dot-sensitized solar cell
journal, January 2011


Lead Iodide Perovskite Sensitized All-Solid-State Submicron Thin Film Mesoscopic Solar Cell with Efficiency Exceeding 9%
journal, August 2012


High-performance photovoltaic perovskite layers fabricated through intramolecular exchange
journal, May 2015


High-efficiency solution-processed perovskite solar cells with millimeter-scale grains
journal, January 2015


Origin and elimination of photocurrent hysteresis by fullerene passivation in CH3NH3PbI3 planar heterojunction solar cells
journal, December 2014


High-Efficiency Solution-Processed Planar Perovskite Solar Cells with a Polymer Hole Transport Layer
journal, December 2014


Growth of CH3NH3PbI3 cuboids with controlled size for high-efficiency perovskite solar cells
journal, August 2014


Detailed Balance Limit of Efficiency of p‐n Junction Solar Cells
journal, March 1961


Controllable Perovskite Crystallization at a Gas–Solid Interface for Hole Conductor-Free Solar Cells with Steady Power Conversion Efficiency over 10%
journal, November 2014


Interface engineering of highly efficient perovskite solar cells
journal, July 2014


Anomalous Hysteresis in Perovskite Solar Cells
journal, April 2014


Impedance Spectroscopic Analysis of Lead Iodide Perovskite-Sensitized Solid-State Solar Cells
journal, December 2013


Giant switchable photovoltaic effect in organometal trihalide perovskite devices
journal, December 2014


Synthesis and crystal chemistry of the hybrid perovskite (CH3NH3)PbI3 for solid-state sensitised solar cell applications
journal, January 2013


Grain-Boundary-Enhanced Carrier Collection in CdTe Solar Cells
journal, April 2014


Elucidating the charge carrier separation and working mechanism of CH3NH3PbI3−xClx perovskite solar cells
journal, March 2014


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journal, August 2016


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journal, May 2016


Grain boundary dominated ion migration in polycrystalline organic–inorganic halide perovskite films
journal, January 2016


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journal, February 2018


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journal, January 2018


Impact of grain boundaries on efficiency and stability of organic-inorganic trihalide perovskites
journal, December 2017


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journal, April 2018


Microstructural investigation of a compact TiO 2 layer for improvement of perovskite solar cells
journal, July 2019


Single Crystal Perovskite Solar Cells: Development and Perspectives
journal, November 2019


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


Bulk heterojunction perovskite–PCBM solar cells with high fill factor
journal, February 2016


The synergistic effect of H 2 O and DMF towards stable and 20% efficiency inverted perovskite solar cells
journal, January 2017


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journal, January 2016


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journal, July 2016


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


Processing‐Performance Evolution of Perovskite Solar Cells: From Large Grain Polycrystalline Films to Single Crystals
journal, April 2020


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journal, January 2017


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journal, May 2019


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journal, January 2016


Spatially segregated free-carrier and exciton populations in individual lead halide perovskite grains
journal, March 2017


The Effects of Electronic Impurities and Electron-Hole Recombination Dynamics on Large-Grain Organic-Inorganic Perovskite Photovoltaic Efficiencies
journal, April 2016


Wafer-scale single-crystal perovskite patterned thin films based on geometrically-confined lateral crystal growth
journal, July 2017


Low thermal budget, photonic-cured compact TiO 2 layers for high-efficiency perovskite solar cells
journal, January 2016


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journal, October 2016


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journal, January 2016


Monolithic perovskite/silicon-heterojunction tandem solar cells processed at low temperature
journal, January 2016


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journal, August 2018


Air-processed mixed-cation Cs 0.15 FA 0.85 PbI 3 planar perovskite solar cells derived from a PbI 2 –CsI–FAI intermediate complex
journal, January 2018


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


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journal, January 2019


The Relationship between Chemical Flexibility and Nanoscale Charge Collection in Hybrid Halide Perovskites
journal, March 2018


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


Mechanism of biphasic charge recombination and accumulation in TiO 2 mesoporous structured perovskite solar cells
journal, January 2016