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Title: Defect Passivation of Organic–Inorganic Hybrid Perovskites by Diammonium Iodide toward High-Performance Photovoltaic Devices

Abstract

The polycrystalline feature of solutionprocessed perovskite film and its ionic nature inevitably incur substantial crystallographic defects, especially at the film surface and the grain boundaries (GBs). Here, a simple defect passivation method was exploited by post-treating CH 3NH 3PbI 3 (MAPbI 3) film with a rationally selected diammonium iodide. The molecular structure of the used diammonium iodide was discovered to play a critical role in affecting the phase purity of treated MAPbI 3. Both NH 3I(CH 2) 4NH 3I and NH 3I(CH 2) 2O(CH 2) 2NH 3I (EDBE) induce three-dimensional (3D) to two-dimensional (2D) perovskite phase transformation during the treatment while only NH 3I(CH 2) 8NH 3I (C 8) successfully passivates perovskite surface and GBs without forming 2D perovskite because of the elevated activation energy arising from its unique anti-gauche isomerization. In conclusion, defect passivation of MAPbI 3 was clearly confirmed by scanning Kelvin probe microscopy (SKPM) and time-resolved photoluminescence (TRPL) studies, which results in the reduced recombination loss in derived devices. Consequently, the perovskite solar cell with C 8 passivation showed a much improved power conversion efficiency (PCE) of 17.60% compared to the control device PCE of 14.64%.

Authors:
 [1];  [1];  [1];  [1];  [2]
  1. Univ. of Washington, Seattle, WA (United States). Dept. of Materials Science and Engineering
  2. Univ. of Washington, Seattle, WA (United States). Dept. of Materials Science and Engineering; Univ. of Washington, Seattle, WA (United States). Dept. of Chemistry
Publication Date:
Research Org.:
Univ. of Washington, Seattle, WA (United States)
Sponsoring Org.:
USDOE Office of Energy Efficiency and Renewable Energy (EERE); National Science Foundation (NSF); US Department of the Navy, Office of Naval Research (ONR); Asian Office of Aerospace R&D
Contributing Org.:
Collaborative Innovation Center of Suzhou Nano Science and Technology; Boeing-Johnson Foundation
OSTI Identifier:
1343582
Report Number(s):
DOE-UW-Jen-16
Journal ID: ISSN 2380-8195
Grant/Contract Number:
EE0006710; DMR-1608279; N00014-14-1- 0246; FA2386-15-1-410
Resource Type:
Journal Article: Accepted Manuscript
Journal Name:
ACS Energy Letters
Additional Journal Information:
Journal Volume: 1; Journal Issue: 4; Journal ID: ISSN 2380-8195
Publisher:
American Chemical Society (ACS)
Country of Publication:
United States
Language:
English
Subject:
14 SOLAR ENERGY; 36 MATERIALS SCIENCE

Citation Formats

Zhao, Ting, Chueh, Chu-Chen, Chen, Qi, Rajagopal, Adharsh, and Jen, Alex K. -Y.. Defect Passivation of Organic–Inorganic Hybrid Perovskites by Diammonium Iodide toward High-Performance Photovoltaic Devices. United States: N. p., 2016. Web. doi:10.1021/acsenergylett.6b00327.
Zhao, Ting, Chueh, Chu-Chen, Chen, Qi, Rajagopal, Adharsh, & Jen, Alex K. -Y.. Defect Passivation of Organic–Inorganic Hybrid Perovskites by Diammonium Iodide toward High-Performance Photovoltaic Devices. United States. doi:10.1021/acsenergylett.6b00327.
Zhao, Ting, Chueh, Chu-Chen, Chen, Qi, Rajagopal, Adharsh, and Jen, Alex K. -Y.. Mon . "Defect Passivation of Organic–Inorganic Hybrid Perovskites by Diammonium Iodide toward High-Performance Photovoltaic Devices". United States. doi:10.1021/acsenergylett.6b00327. https://www.osti.gov/servlets/purl/1343582.
@article{osti_1343582,
title = {Defect Passivation of Organic–Inorganic Hybrid Perovskites by Diammonium Iodide toward High-Performance Photovoltaic Devices},
author = {Zhao, Ting and Chueh, Chu-Chen and Chen, Qi and Rajagopal, Adharsh and Jen, Alex K. -Y.},
abstractNote = {The polycrystalline feature of solutionprocessed perovskite film and its ionic nature inevitably incur substantial crystallographic defects, especially at the film surface and the grain boundaries (GBs). Here, a simple defect passivation method was exploited by post-treating CH3NH3PbI3 (MAPbI3) film with a rationally selected diammonium iodide. The molecular structure of the used diammonium iodide was discovered to play a critical role in affecting the phase purity of treated MAPbI3. Both NH3I(CH2)4NH3I and NH3I(CH2)2O(CH2)2NH3I (EDBE) induce three-dimensional (3D) to two-dimensional (2D) perovskite phase transformation during the treatment while only NH3I(CH2)8NH3I (C8) successfully passivates perovskite surface and GBs without forming 2D perovskite because of the elevated activation energy arising from its unique anti-gauche isomerization. In conclusion, defect passivation of MAPbI3 was clearly confirmed by scanning Kelvin probe microscopy (SKPM) and time-resolved photoluminescence (TRPL) studies, which results in the reduced recombination loss in derived devices. Consequently, the perovskite solar cell with C8 passivation showed a much improved power conversion efficiency (PCE) of 17.60% compared to the control device PCE of 14.64%.},
doi = {10.1021/acsenergylett.6b00327},
journal = {ACS Energy Letters},
number = 4,
volume = 1,
place = {United States},
year = {Mon Sep 12 00:00:00 EDT 2016},
month = {Mon Sep 12 00:00:00 EDT 2016}
}

Journal Article:
Free Publicly Available Full Text
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Cited by: 19works
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  • We report on the carrier-rotor coupling effect in perovskite organic-inorganic hybrid lead iodide (CH3NH3PbI3) compounds discovered by isotope effects. Deuterated organic-inorganic perovskite compounds including CH3ND3PbI3, CD3NH3PbI3, and CD3ND3PbI3 were synthesized. Devices made from regular CH3NH3PbI3 and deuterated CH3ND3PbI3 exhibit comparable performance in band gap, current-voltage, carrier mobility, and power conversion efficiency. However, a time-resolved photoluminescence (TRPL) study reveals that CH3NH3PbI3 exhibits notably longer carrier lifetime than that of CH3ND3PbI3, in both thin-film and single-crystal formats. Furthermore, the comparison in carrier lifetime between CD3NH3PbI3 and CH3ND3PbI3 single crystals suggests that vibrational modes in methylammonium (MA+) have little impact on carrier lifetime.more » In contrast, the fully deuterated compound CD3ND3PbI3 reconfirmed the trend of decreasing carrier lifetime upon the increasing moment of inertia of cationic MA+. Polaron model elucidates the electron-rotor interaction.« less
  • We report on the carrier-rotor coupling effect in perovskite organic-inorganic hybrid lead iodide (CH3NH3PbI3) compounds discovered by isotope effects. Deuterated organic-inorganic perovskite compounds including CH3ND3PbI3, CD3NH3PbI3, and CD3ND3PbI3 were synthesized. Devices made from regular CH3NH3PbI3 and deuterated CH3ND3PbI3 exhibit comparable performance in band gap, current-voltage, carrier mobility, and power conversion efficiency. However, a time-resolved photoluminescence (TRPL) study reveals that CH3NH3PbI3 exhibits notably longer carrier lifetime than that of CH3ND3PbI3, in both thin-film and single crystal formats. Furthermore, the comparison in carrier lifetime between CD3NH3PbI3 and CH3ND3PbI3 single crystals suggests that vibrational modes in methylammonium (MA(+)) have little impact on carriermore » lifetime. In contrast, the fully deuterated compound CD3ND3PbI3 reconfirmed the trend of decreasing carrier lifetime upon the increasing moment of inertia of cationic MA(+). Polaron model elucidates the electron-rotor interaction.« less
  • High-bandgap mixed-halide hybrid perovskites have higher open-circuit voltage deficits and lower carrier diffusion lengths than their lower-bandgap counterparts. We have developed a ligand-assisted crystallization (LAC) technique that introduces additives in situ during the solvent wash and developed a new method to dynamically measure the absolute intensity steady-state photoluminescence and the mean carrier diffusion length simultaneously. The measurements reveal four distinct regimes of material changes and show that photoluminescence brightening often coincides with losses in carrier transport, such as in degradation or phase segregation. Further, the measurements enabled optimization of LAC on the 1.75 eV bandgap FA 0.83Cs 0.17Pb(I 0.66Br 0.34)more » 3, resulting in an enhancement of the photoluminescence quantum yield (PLQY) of over an order of magnitude, an increase of 80 meV in the quasi-Fermi level splitting (to 1.29 eV), an increase in diffusion length by a factor of 3.5 (to over 1 μm), and enhanced open-circuit voltage and short-circuit current from photovoltaics fabricated from the LAC-treated films.« less
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  • High-bandgap mixed-halide hybrid perovskites have higher open-circuit voltage deficits and lower carrier diffusion lengths than their lower-bandgap counterparts. We have developed a ligand-assisted crystallization (LAC) technique that introduces additives in situ during the solvent wash and developed a new method to dynamically measure the absolute intensity steady-state photoluminescence and the mean carrier diffusion length simultaneously. The measurements reveal four distinct regimes of material changes and show that photoluminescence brightening often coincides with losses in carrier transport, such as in degradation or phase segregation. Further, the measurements enabled optimization of LAC on the 1.75 eV bandgap FA 0.83Cs 0.17Pb(I 0.66Br 0.34)more » 3, resulting in an enhancement of the photoluminescence quantum yield (PLQY) of over an order of magnitude, an increase of 80 meV in the quasi-Fermi level splitting (to 1.29 eV), an increase in diffusion length by a factor of 3.5 (to over 1 μm), and enhanced open-circuit voltage and short-circuit current from photovoltaics fabricated from the LAC-treated films.« less
  • High-bandgap mixed-halide hybrid perovskites have higher open-circuit voltage deficits and lower carrier diffusion lengths than their lower-bandgap counterparts. We have developed a ligand-assisted crystallization (LAC) technique that introduces additives in situ during the solvent wash and developed a new method to dynamically measure the absolute intensity steady-state photoluminescence and the mean carrier diffusion length simultaneously. The measurements reveal four distinct regimes of material changes and show that photoluminescence brightening often coincides with losses in carrier transport, such as in degradation or phase segregation. Further, the measurements enabled optimization of LAC on the 1.75 eV bandgap FA 0.83Cs 0.17Pb(I 0.66Br 0.34)more » 3, resulting in an enhancement of the photoluminescence quantum yield (PLQY) of over an order of magnitude, an increase of 80 meV in the quasi-Fermi level splitting (to 1.29 eV), an increase in diffusion length by a factor of 3.5 (to over 1 μm), and enhanced open-circuit voltage and short-circuit current from photovoltaics fabricated from the LAC-treated films.« less