GeI 2 additive for high optoelectronic quality CsPbI 3 quantum dots and their application in photovoltaic devices

Feng Liu, Chao Ding, Yaohong Zhang, Taichi Kamisaka, Qian Zhao, Joseph M. Luther, Taro Toyoda, Shuzi Hayase, Takashi Minemoto, Kenji Yoshino, Bing Zhang, Songyuan Dai, Junke Jiang, Shuxia Tao, Qing Shen (Corresponding author)

Research output: Contribution to journalArticleAcademicpeer-review

18 Citations (Scopus)
1 Downloads (Pure)

Abstract

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.
Original languageEnglish
Pages (from-to)798-807
Number of pages10
JournalChemistry of Materials
Volume31
Issue number3
DOIs
Publication statusPublished - 12 Feb 2019

Fingerprint

Optoelectronic devices
Semiconductor quantum dots
Quantum yield
Iodine
Photoluminescence
Metal halides
Carrier lifetime
Chemical stability
Stoichiometry
Perovskite
Conversion efficiency
Solar cells
Salts
Ions

Cite this

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. / GeI 2 additive for high optoelectronic quality CsPbI 3 quantum dots and their application in photovoltaic devices. In: Chemistry of Materials. 2019 ; Vol. 31, No. 3. pp. 798-807.
@article{4114eed02c254db08dfe01a0d0bafbbe,
title = "GeI 2 additive for high optoelectronic quality CsPbI 3 quantum dots and their application in photovoltaic devices",
abstract = "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.",
author = "Feng Liu and Chao Ding and Yaohong Zhang and Taichi Kamisaka and Qian Zhao and Luther, {Joseph M.} and Taro Toyoda and Shuzi Hayase and Takashi Minemoto and Kenji Yoshino and Bing Zhang and Songyuan Dai and Junke Jiang and Shuxia Tao and Qing Shen",
year = "2019",
month = "2",
day = "12",
doi = "10.1021/acs.chemmater.8b03871",
language = "English",
volume = "31",
pages = "798--807",
journal = "Chemistry of Materials",
issn = "0897-4756",
publisher = "American Chemical Society",
number = "3",

}

Liu, F, Ding, C, Zhang, Y, Kamisaka, T, Zhao, Q, Luther, JM, Toyoda, T, Hayase, S, Minemoto, T, Yoshino, K, Zhang, B, Dai, S, Jiang, J, Tao, S & Shen, Q 2019, 'GeI 2 additive for high optoelectronic quality CsPbI 3 quantum dots and their application in photovoltaic devices', Chemistry of Materials, vol. 31, no. 3, pp. 798-807. https://doi.org/10.1021/acs.chemmater.8b03871

GeI 2 additive for high optoelectronic quality CsPbI 3 quantum dots and their application in photovoltaic devices. / 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 (Corresponding author).

In: Chemistry of Materials, Vol. 31, No. 3, 12.02.2019, p. 798-807.

Research output: Contribution to journalArticleAcademicpeer-review

TY - JOUR

T1 - GeI 2 additive for high optoelectronic quality CsPbI 3 quantum dots and their application in photovoltaic devices

AU - Liu, Feng

AU - Ding, Chao

AU - Zhang, Yaohong

AU - Kamisaka, Taichi

AU - Zhao, Qian

AU - Luther, Joseph M.

AU - Toyoda, Taro

AU - Hayase, Shuzi

AU - Minemoto, Takashi

AU - Yoshino, Kenji

AU - Zhang, Bing

AU - Dai, Songyuan

AU - Jiang, Junke

AU - Tao, Shuxia

AU - Shen, Qing

PY - 2019/2/12

Y1 - 2019/2/12

N2 - 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.

AB - 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.

UR - http://www.scopus.com/inward/record.url?scp=85061654813&partnerID=8YFLogxK

U2 - 10.1021/acs.chemmater.8b03871

DO - 10.1021/acs.chemmater.8b03871

M3 - Article

VL - 31

SP - 798

EP - 807

JO - Chemistry of Materials

JF - Chemistry of Materials

SN - 0897-4756

IS - 3

ER -