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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 Laboratory (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:
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. 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, and Xiao, Kai. Thu . "Perovskite Solar Cells with Near 100% Internal Quantum Efficiency Based on Large Single Crystalline Grains and Vertical Bulk Heterojunctions". United States. doi: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},
journal = {Journal of the American Chemical Society},
number = 29,
volume = 137,
place = {United States},
year = {2015},
month = {7}
}

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Works referencing / citing this record:

Controllable growth of bulk cubic-phase CH 3 NH 3 PbI 3 single crystal with exciting room-temperature stability
journal, January 2016

  • Luan, Mengyu; Song, Junling; Wei, Xiangfeng
  • CrystEngComm, Vol. 18, Issue 28
  • DOI: 10.1039/c6ce00375c

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

  • Albrecht, Steve; Saliba, Michael; Correa Baena, Juan Pablo
  • Energy & Environmental Science, Vol. 9, Issue 1
  • DOI: 10.1039/c5ee02965a

Molecular modulator for stable inverted planar perovskite solar cells with efficiency enhanced by interface engineering
journal, January 2019

  • Zhao, Z. Q.; You, S.; Huang, J.
  • Journal of Materials Chemistry C, Vol. 7, Issue 31
  • DOI: 10.1039/c9tc03259b

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

  • Albrecht, Steve; Saliba, Michael; Correa Baena, Juan Pablo
  • Energy & Environmental Science, Vol. 9, Issue 1
  • DOI: 10.1039/c5ee02965a

Boosting the performance of planar heterojunction perovskite solar cell by controlling the precursor purity of perovskite materials
journal, January 2016

  • Chang, Jingjing; Zhu, Hai; Li, Bichen
  • Journal of Materials Chemistry A, Vol. 4, Issue 3
  • DOI: 10.1039/c5ta08398b

Controllable growth of bulk cubic-phase CH 3 NH 3 PbI 3 single crystal with exciting room-temperature stability
journal, January 2016

  • Luan, Mengyu; Song, Junling; Wei, Xiangfeng
  • CrystEngComm, Vol. 18, Issue 28
  • DOI: 10.1039/c6ce00375c

Molecular modulator for stable inverted planar perovskite solar cells with efficiency enhanced by interface engineering
journal, January 2019

  • Zhao, Z. Q.; You, S.; Huang, J.
  • Journal of Materials Chemistry C, Vol. 7, Issue 31
  • DOI: 10.1039/c9tc03259b

Elucidating the charge carrier transport and extraction in planar heterojunction perovskite solar cells by Kelvin probe force microscopy
journal, January 2016

  • Chang, Jingjing; Xiao, Juanxiu; Lin, Zhenhua
  • Journal of Materials Chemistry A, Vol. 4, Issue 44
  • DOI: 10.1039/c6ta05350e

CH 3 NH 3 PbI 3 grain growth and interfacial properties in meso-structured perovskite solar cells fabricated by two-step deposition
journal, January 2017