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Title: Perovskite Quantum Dot Photovoltaic Materials beyond the Reach of Thin Films: Full-Range Tuning of A-Site Cation Composition

Abstract

We present a cation-exchange approach for tunable A-site alloys of cesium (Cs+) and formamidinium (FA+) lead triiodide perovskite nanocrystals that enables the formation of compositions spanning the complete range of Cs1-xFAxPbI3, unlike thin-film alloys or the direct synthesis of alloyed perovskite nanocrystals. These materials show bright and finely tunable emission in the red and near-infrared range between 650 and 800 nm. The activation energy for the miscibility between Cs+ and FA+ is measured (~0.65 eV) and is shown to be higher than reported for X-site exchange in lead halide perovskites. We use these alloyed colloidal perovskite quantum dots to fabricate photovoltaic devices. In addition to the expanded compositional range for Cs1-xFAxPbI3 materials, the quantum dot solar cells exhibit high open-circuit voltage (VOC) with a lower loss than the thin-film perovskite devices of similar compositions.

Authors:
ORCiD logo [1];  [2];  [1]; ORCiD logo [1];  [3];  [1];  [1]; ORCiD logo [1]; ORCiD logo [1]; ORCiD logo [1]
  1. National Renewable Energy Lab. (NREL), Golden, CO (United States)
  2. National Renewable Energy Lab. (NREL), Golden, CO (United States); Nankai Univ., Tianjin (China)
  3. National Renewable Energy Lab. (NREL), Golden, CO (United States); Univ. of Colorado, Boulder, CO (United States)
Publication Date:
Research Org.:
Energy Frontier Research Centers (EFRC) (United States). Center for Advanced Solar Photophysics (CASP); National Renewable Energy Lab. (NREL), Golden, CO (United States)
Sponsoring Org.:
USDOE Office of Energy Efficiency and Renewable Energy (EERE), Renewable Power Office. Solar Energy Technologies Office
OSTI Identifier:
1476707
Report Number(s):
NREL/JA-5900-71956
Journal ID: ISSN 1936-0851
Grant/Contract Number:  
AC36-08GO28308
Resource Type:
Accepted Manuscript
Journal Name:
ACS Nano
Additional Journal Information:
Journal Volume: 12; Journal Issue: 10; Journal ID: ISSN 1936-0851
Publisher:
American Chemical Society (ACS)
Country of Publication:
United States
Language:
English
Subject:
14 SOLAR ENERGY; 77 NANOSCIENCE AND NANOTECHNOLOGY; A-site alloying; cation exchange; lead halide; nanocrystals; perovskites; quantum dots; solar cells

Citation Formats

Hazarika, Abhijit, Zhao, Qian, Gaulding, E. Ashley, Christians, Jeffrey A., Dou, Benjia, Marshall, Ashley R., Moot, Taylor, Berry, Joseph J., Johnson, Justin C., and Luther, Joseph M. Perovskite Quantum Dot Photovoltaic Materials beyond the Reach of Thin Films: Full-Range Tuning of A-Site Cation Composition. United States: N. p., 2018. Web. https://doi.org/10.1021/acsnano.8b05555.
Hazarika, Abhijit, Zhao, Qian, Gaulding, E. Ashley, Christians, Jeffrey A., Dou, Benjia, Marshall, Ashley R., Moot, Taylor, Berry, Joseph J., Johnson, Justin C., & Luther, Joseph M. Perovskite Quantum Dot Photovoltaic Materials beyond the Reach of Thin Films: Full-Range Tuning of A-Site Cation Composition. United States. https://doi.org/10.1021/acsnano.8b05555
Hazarika, Abhijit, Zhao, Qian, Gaulding, E. Ashley, Christians, Jeffrey A., Dou, Benjia, Marshall, Ashley R., Moot, Taylor, Berry, Joseph J., Johnson, Justin C., and Luther, Joseph M. Tue . "Perovskite Quantum Dot Photovoltaic Materials beyond the Reach of Thin Films: Full-Range Tuning of A-Site Cation Composition". United States. https://doi.org/10.1021/acsnano.8b05555. https://www.osti.gov/servlets/purl/1476707.
@article{osti_1476707,
title = {Perovskite Quantum Dot Photovoltaic Materials beyond the Reach of Thin Films: Full-Range Tuning of A-Site Cation Composition},
author = {Hazarika, Abhijit and Zhao, Qian and Gaulding, E. Ashley and Christians, Jeffrey A. and Dou, Benjia and Marshall, Ashley R. and Moot, Taylor and Berry, Joseph J. and Johnson, Justin C. and Luther, Joseph M.},
abstractNote = {We present a cation-exchange approach for tunable A-site alloys of cesium (Cs+) and formamidinium (FA+) lead triiodide perovskite nanocrystals that enables the formation of compositions spanning the complete range of Cs1-xFAxPbI3, unlike thin-film alloys or the direct synthesis of alloyed perovskite nanocrystals. These materials show bright and finely tunable emission in the red and near-infrared range between 650 and 800 nm. The activation energy for the miscibility between Cs+ and FA+ is measured (~0.65 eV) and is shown to be higher than reported for X-site exchange in lead halide perovskites. We use these alloyed colloidal perovskite quantum dots to fabricate photovoltaic devices. In addition to the expanded compositional range for Cs1-xFAxPbI3 materials, the quantum dot solar cells exhibit high open-circuit voltage (VOC) with a lower loss than the thin-film perovskite devices of similar compositions.},
doi = {10.1021/acsnano.8b05555},
journal = {ACS Nano},
number = 10,
volume = 12,
place = {United States},
year = {2018},
month = {9}
}

Journal Article:
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Cited by: 18 works
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Figures / Tables:

Figure 1 Figure 1: A-site ion exchange to form phase stable Cs1−xFAxPbI3 NCs. (A) Schematic diagram showing the cross-exchange of Cs+ and FA+ ions between CsPbI3 and FAPbI3 perovskite NCs. (B) Goldschmidt tolerance factor as a function of FA+ ion concentration shows that all compositions are expected to be phase-stable (the purplemore » region in the plot). Top axis shows the effective or average A-site radius. (C) PL emission spectra depicting how CsPbI3 and FAPbI3 NCs convert into alloyed NCs; the dashed curve indicates the emission profile of one of the early stages of alloying.« less

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