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Title: GeI 2 Additive for High Optoelectronic Quality CsPbI 3 Quantum Dots and Their Application in Photovoltaic Devices

Abstract

Trioctylphosphine (TOP)-based syntheses of CsPbI 3 perovskite quantum dots (QDs) yield unprecedented high photoluminescence quantum yield (PL QY), lower Stokes shifts, and longer carrier lifetimes due to their enhanced crystallinity. This synthetic route relies on a heavily Pb-rich condition or a large Pb:Cs molar ratio in precursor solution to produce QDs with appropriate stoichiometry as well as to guarantee a good colloidal stability. The high Pb condition is achieved by a high concentration of PbI 2 prepared in TOP. Here we find such Pb-rich strategies can be avoided by providing additional iodine ions using other metal halide salts. In particular GeI 2, which contrary to PbI 2, readily dissolves in TOP. CsPbI 3 QDs prepared using PbI 2/GeI 2 combination show near-unity PL QY and improved chemical stability compared to the previous synthetic route. Furthermore, we find no sign of Ge incorporation in the QDs (compositionally or energetically). The ensuing QD solar cells deliver power conversion efficiency of 12.15% and retain 85% of its peak performance after storage over 90 days. The PbI 2/GeI 2 dual-source iodine synthetic approach presented here represents a more rational and robust route to high-quality CsPbI 3 QDs. to guarantee a good colloidal stability. Themore » high Pb condition is achieved by a high concentration of PbI2 prepared in TOP. Here we find such Pb-rich strategies can be avoided by providing additional iodine ions using other metal halide salts. In particular GeI 2, which contrary to PbI 2, readily dissolves in TOP. CsPbI 3 QDs prepared using PbI 2/GeI 2 combination show near-unity PL QY and improved chemical stability compared to the previous synthetic route. Furthermore, we find no sign of Ge incorporation in the QDs (compositionally or energetically). The ensuing QD solar cells deliver power conversion efficiency of 12.15% and retain 85% of its peak performance after storage over 90 days. The PbI 2/GeI 2 dual-source iodine synthetic approach presented here represents a more rational and robust route to high-quality CsPbI 3 QDs.« less

Authors:
 [1];  [1];  [1];  [1];  [2]; ORCiD logo [3];  [1];  [4];  [5];  [6];  [7];  [7];  [8];  [8];  [1]
  1. Univ. of Electro-Communications, Tokyo (Japan)
  2. National Renewable Energy Lab. (NREL), Golden, CO (United States); Nankai Univ. (China)
  3. National Renewable Energy Lab. (NREL), Golden, CO (United States)
  4. Kyushu Inst. of Technology, Kitakyushu (Japan)
  5. Ritsumeikan Univ., Shiga (Japan)
  6. Miyazaki Univ. (Japan)
  7. North China Electric Power Univ., Beijing (China)
  8. Eindhoven Univ. of Technology (Netherlands)
Publication Date:
Research Org.:
National Renewable Energy Lab. (NREL), Golden, CO (United States)
Sponsoring Org.:
USDOE National Renewable Energy Laboratory (NREL), Laboratory Directed Research and Development (LDRD) Program
OSTI Identifier:
1513189
Report Number(s):
NREL/JA-5900-71882
Journal ID: ISSN 0897-4756
Grant/Contract Number:  
AC36-08GO28308
Resource Type:
Accepted Manuscript
Journal Name:
Chemistry of Materials
Additional Journal Information:
Journal Volume: 31; Journal Issue: 3; Journal ID: ISSN 0897-4756
Publisher:
American Chemical Society (ACS)
Country of Publication:
United States
Language:
English
Subject:
14 SOLAR ENERGY; 36 MATERIALS SCIENCE; quantum dots; photoluminescence quantum yield; Gel2

Citation Formats

Liu, Feng, Ding, Chao, Zhang, Yaohong, Kamisaka, Taichi, Zhao, Qian, Luther, Joseph M, Toyoda, Taro, Hayase, Shuzi, Minemoto, Takashi, Yoshino, Kenji, Zhang, Bing, Dai, Songyuan, Jiang, Junke, Tao, Shuxia, and Shen, Qing. GeI2 Additive for High Optoelectronic Quality CsPbI3 Quantum Dots and Their Application in Photovoltaic Devices. United States: N. p., 2019. Web. doi:10.1021/acs.chemmater.8b03871.
Liu, Feng, Ding, Chao, Zhang, Yaohong, Kamisaka, Taichi, Zhao, Qian, Luther, Joseph M, Toyoda, Taro, Hayase, Shuzi, Minemoto, Takashi, Yoshino, Kenji, Zhang, Bing, Dai, Songyuan, Jiang, Junke, Tao, Shuxia, & Shen, Qing. GeI2 Additive for High Optoelectronic Quality CsPbI3 Quantum Dots and Their Application in Photovoltaic Devices. United States. doi:10.1021/acs.chemmater.8b03871.
Liu, Feng, Ding, Chao, Zhang, Yaohong, Kamisaka, Taichi, Zhao, Qian, Luther, Joseph M, Toyoda, Taro, Hayase, Shuzi, Minemoto, Takashi, Yoshino, Kenji, Zhang, Bing, Dai, Songyuan, Jiang, Junke, Tao, Shuxia, and Shen, Qing. Mon . "GeI2 Additive for High Optoelectronic Quality CsPbI3 Quantum Dots and Their Application in Photovoltaic Devices". United States. doi:10.1021/acs.chemmater.8b03871.
@article{osti_1513189,
title = {GeI2 Additive for High Optoelectronic Quality CsPbI3 Quantum Dots and Their Application in Photovoltaic Devices},
author = {Liu, Feng and Ding, Chao and Zhang, Yaohong and Kamisaka, Taichi and Zhao, Qian and Luther, Joseph M and Toyoda, Taro and Hayase, Shuzi and Minemoto, Takashi and Yoshino, Kenji and Zhang, Bing and Dai, Songyuan and Jiang, Junke and Tao, Shuxia and Shen, Qing},
abstractNote = {Trioctylphosphine (TOP)-based syntheses of CsPbI3 perovskite quantum dots (QDs) yield unprecedented high photoluminescence quantum yield (PL QY), lower Stokes shifts, and longer carrier lifetimes due to their enhanced crystallinity. This synthetic route relies on a heavily Pb-rich condition or a large Pb:Cs molar ratio in precursor solution to produce QDs with appropriate stoichiometry as well as to guarantee a good colloidal stability. The high Pb condition is achieved by a high concentration of PbI2 prepared in TOP. Here we find such Pb-rich strategies can be avoided by providing additional iodine ions using other metal halide salts. In particular GeI2, which contrary to PbI2, readily dissolves in TOP. CsPbI3 QDs prepared using PbI2/GeI2 combination show near-unity PL QY and improved chemical stability compared to the previous synthetic route. Furthermore, we find no sign of Ge incorporation in the QDs (compositionally or energetically). The ensuing QD solar cells deliver power conversion efficiency of 12.15% and retain 85% of its peak performance after storage over 90 days. The PbI2/GeI2 dual-source iodine synthetic approach presented here represents a more rational and robust route to high-quality CsPbI3 QDs. to guarantee a good colloidal stability. The high Pb condition is achieved by a high concentration of PbI2 prepared in TOP. Here we find such Pb-rich strategies can be avoided by providing additional iodine ions using other metal halide salts. In particular GeI2, which contrary to PbI2, readily dissolves in TOP. CsPbI3 QDs prepared using PbI2/GeI2 combination show near-unity PL QY and improved chemical stability compared to the previous synthetic route. Furthermore, we find no sign of Ge incorporation in the QDs (compositionally or energetically). The ensuing QD solar cells deliver power conversion efficiency of 12.15% and retain 85% of its peak performance after storage over 90 days. The PbI2/GeI2 dual-source iodine synthetic approach presented here represents a more rational and robust route to high-quality CsPbI3 QDs.},
doi = {10.1021/acs.chemmater.8b03871},
journal = {Chemistry of Materials},
number = 3,
volume = 31,
place = {United States},
year = {2019},
month = {1}
}

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