Lead Halide Perovskite Nanocrystals with Low Inhomogeneous Broadening and High Coherent Fraction through Dicationic Ligand Engineering ?

被引:16
作者
Ginterseder, Matthias [1 ,2 ]
Sun, Weiwei [1 ]
Shcherbakov-Wu, Wenbi [3 ]
McIsaac, Alexandra R. [1 ,2 ]
Berkinsky, David B. [1 ]
Kaplan, Alexander E. K. [1 ]
Wang, Lili [1 ,4 ]
Krajewska, Chantalle [1 ]
Sverko, Tara [1 ]
Perkinson, Collin F. [1 ]
Utzat, Hendrik [1 ,2 ]
Tisdale, William A. [1 ]
Van Voorhis, Troy [1 ]
Bawendi, Moungi G. [1 ]
机构
[1] MIT, Dept Chem, Cambridge, MA 02139 USA
[2] Univ Calif Berkeley, Dept Chem, Berkeley, CA 94720 USA
[3] MIT, Dept Chem Engn, Cambridge, MA 02139 USA
[4] Emory Univ, Dept Chem, Atlanta, GA 30322 USA
基金
美国国家科学基金会;
关键词
colloidal quantum dots; lead halide perovskites; ligand engineering; inhomogeneous broadening; Stokes shift; coherent emission; QUANTUM DOTS; LUMINESCENT; PASSIVATION; ORIGIN; CSPBX3; BRIGHT; BR;
D O I
10.1021/acs.nanolett.2c03354
中图分类号
O6 [化学];
学科分类号
0703 ;
摘要
Lead halide perovskite nanocrystals (LHP NCs) are an emerging materials system with broad potential applications, including as emitters of quantum light. We apply design principles aimed at the structural optimization of surface ligand species for CsPbBr3 NCs, leading us to the study of LHP NCs with dicationic quaternary ammonium bromide ligands. Through the selection of linking groups and aliphatic backbones guided by experiments and computational support, we demonstrate consistently narrow photoluminescence line shapes with a full-width-at-half-maximum below 70 meV. We observe bulk-like Stokes shifts throughout our range of particle sizes, from 7 to 16 nm. At cryogenic temperatures, we find sub-200 ps lifetimes, significant photon coherence, and the fraction of photons emitted into the coherent channel increasing markedly to 86%. A 4-fold reduction in inhomogeneous broadening from previous work paves the way for the integration of LHP NC emitters into nanophotonic architectures to enable advanced quantum optical investigation.
引用
收藏
页码:1128 / 1134
页数:7
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