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Title: Enhanced Open-Circuit Voltage of Wide-Bandgap Perovskite Photovoltaics by Using Alloyed (FA1–xCsx)Pb(I1–xBrx)3 Quantum Dots

Abstract

We report a detailed study on APbX3 (A=Formamidinium (FA+), Cs+; X=I-, Br-) perovskite quantum dots (PQDs) with combined A- and X-site alloying that exhibit, both, a wide bandgap and high open circuit voltage (Voc) for the application of a potential top cell in tandem junction photovoltaic (PV) devices. The nanocrystal alloying affords control over the optical bandgap and is readily achieved by solution-phase cation and anion exchange between previously synthesized FAPbI3 and CsPbBr3 PQDs. Increasing only the Br- content of the PQDs widens the bandgap but results in shorter carrier lifetimes and associated Voc losses in devices. These deleterious effects can be mitigated by replacing Cs+ with FA+, resulting in wide bandgap PQD absorbers with improved charge-carrier mobility and PVs with higher Voc. Although further device optimization is required, these results demonstrate the potential of FA1–xCsx)Pb(I1–xBrx)3 PQDs for wide bandgap perovskite PVs with high Voc.

Authors:
 [1];  [1];  [1];  [1];  [1];  [2];  [2]; ORCiD logo [1];  [2]; ORCiD logo [1]
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  1. National Renewable Energy Laboratory (NREL), Golden, CO (United States)
  2. University of Texas, Austin
Publication Date:
Research Org.:
National Renewable Energy Lab. (NREL), Golden, CO (United States)
Sponsoring Org.:
USDOE Office of Science (SC), Workforce Development for Teachers and Scientists (WDTS)
OSTI Identifier:
1544533
Report Number(s):
NREL/JA-5900-73572
Journal ID: ISSN 2380-8195
Grant/Contract Number:  
AC36-08GO28308
Resource Type:
Accepted Manuscript
Journal Name:
ACS Energy Letters
Additional Journal Information:
Journal Volume: 4; Journal Issue: 8; Journal ID: ISSN 2380-8195
Publisher:
American Chemical Society (ACS)
Country of Publication:
United States
Language:
English
Subject:
14 SOLAR ENERGY; 36 MATERIALS SCIENCE; perovskite quantum dots; alloys; photovoltaic devices

Citation Formats

Suri, Mokshin, Hazarika, Abhijit, Larson, Bryon W, Zhao, Qian, Valles Pelarda, Marta, Siegler, Timothy D., Abney, Michael K., Ferguson, Andrew J, Korgel, Brian A., and Luther, Joseph M. Enhanced Open-Circuit Voltage of Wide-Bandgap Perovskite Photovoltaics by Using Alloyed (FA1–xCsx)Pb(I1–xBrx)3 Quantum Dots. United States: N. p., 2019. Web. doi:10.1021/acsenergylett.9b01030.
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Suri, Mokshin, Hazarika, Abhijit, Larson, Bryon W, Zhao, Qian, Valles Pelarda, Marta, Siegler, Timothy D., Abney, Michael K., Ferguson, Andrew J, Korgel, Brian A., & Luther, Joseph M. Enhanced Open-Circuit Voltage of Wide-Bandgap Perovskite Photovoltaics by Using Alloyed (FA1–xCsx)Pb(I1–xBrx)3 Quantum Dots. United States. https://doi.org/10.1021/acsenergylett.9b01030
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Suri, Mokshin, Hazarika, Abhijit, Larson, Bryon W, Zhao, Qian, Valles Pelarda, Marta, Siegler, Timothy D., Abney, Michael K., Ferguson, Andrew J, Korgel, Brian A., and Luther, Joseph M. Tue . "Enhanced Open-Circuit Voltage of Wide-Bandgap Perovskite Photovoltaics by Using Alloyed (FA1–xCsx)Pb(I1–xBrx)3 Quantum Dots". United States. https://doi.org/10.1021/acsenergylett.9b01030. https://www.osti.gov/servlets/purl/1544533.
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@article{osti_1544533,
title = {Enhanced Open-Circuit Voltage of Wide-Bandgap Perovskite Photovoltaics by Using Alloyed (FA1–xCsx)Pb(I1–xBrx)3 Quantum Dots},
author = {Suri, Mokshin and Hazarika, Abhijit and Larson, Bryon W and Zhao, Qian and Valles Pelarda, Marta and Siegler, Timothy D. and Abney, Michael K. and Ferguson, Andrew J and Korgel, Brian A. and Luther, Joseph M},
abstractNote = {We report a detailed study on APbX3 (A=Formamidinium (FA+), Cs+; X=I-, Br-) perovskite quantum dots (PQDs) with combined A- and X-site alloying that exhibit, both, a wide bandgap and high open circuit voltage (Voc) for the application of a potential top cell in tandem junction photovoltaic (PV) devices. The nanocrystal alloying affords control over the optical bandgap and is readily achieved by solution-phase cation and anion exchange between previously synthesized FAPbI3 and CsPbBr3 PQDs. Increasing only the Br- content of the PQDs widens the bandgap but results in shorter carrier lifetimes and associated Voc losses in devices. These deleterious effects can be mitigated by replacing Cs+ with FA+, resulting in wide bandgap PQD absorbers with improved charge-carrier mobility and PVs with higher Voc. Although further device optimization is required, these results demonstrate the potential of FA1–xCsx)Pb(I1–xBrx)3 PQDs for wide bandgap perovskite PVs with high Voc.},
doi = {10.1021/acsenergylett.9b01030},
journal = {ACS Energy Letters},
number = 8,
volume = 4,
place = {United States},
year = {Tue Jul 02 00:00:00 EDT 2019},
month = {Tue Jul 02 00:00:00 EDT 2019}
}
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Journal Article:
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Publisher's Version of Record
https://doi.org/10.1021/acsenergylett.9b01030
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Cited by: 49 works
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Figures / Tables:

Figure 1 Figure 1: A) Crystal models showing the ion exchange process used to generate alloyed PQDs. FA1xCsxPb(I1-xBrx)3 PQDs are generated when dispersions of CsPbBr3 and FAPbI3 PQDs are mixed at 70°C. Room temperature (B) absorbance and (C) PL emission spectra of PQDs with varying FA1-xCsxPb(I1xBrx)3 composition dispersed in octane (excitation wavelengthmore » of 400 nm).« less
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