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

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          Abstract

          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.

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          Author and article information

          Journal
          Nano Lett
          Nano letters
          American Chemical Society (ACS)
          1530-6992
          1530-6984
          Feb 22 2023
          : 23
          : 4
          Affiliations
          [1 ] Department of Chemistry, Massachusetts Institute of Technology, Cambridge, Massachusetts 02139, United States.
          [2 ] Department of Chemical Engineering, Massachusetts Institute of Technology, Cambridge, Massachusetts 02139, United States.
          Article
          10.1021/acs.nanolett.2c03354
          36780509
          373a094b-dc6f-45f4-ad65-883311a25874
          History

          ligand engineering,lead halide perovskites,inhomogeneous broadening,colloidal quantum dots,coherent emission,Stokes shift

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