Optical properties of single CsPbBr3 perovskite quantum dots synthesized by a modified ligand-assisted reprecipitation method

TL;DR

This study demonstrates that a modified ligand-assisted reprecipitation method can produce CsPbBr3 perovskite quantum dots with high optical quality at the single-particle level, comparable to hot-injection synthesis, with enhanced stability and optical properties.

Contribution

The paper introduces a modified LARP synthesis protocol that yields high-quality, stable single CsPbBr3 pQDs with detailed optical characterization, offering an accessible alternative to hot-injection methods.

Findings

High-quality single pQDs with stable emission and minimal spectral diffusion.

Observation of exciton fine structure, phonon replicas, and multiexciton states.

Single photon emission with ~90 ps lifetime and high purity.

Abstract

Colloidal perovskite quantum dots (pQDs) are promising quantum light emitters, and investigations at the single pQD scale have so far relied mostly on hot-injection synthesis, which requires precise temperature control and an inert atmosphere. While alternative synthesis routes under milder conditions are often associated with structural and surface defects that may have limited impact in ensemble measurements, demonstrating high optical quality at the level of individual pQDs constitutes the most stringent benchmark for a new synthesis protocol. Here, we demonstrate that a modified ligand-assisted reprecipitation (LARP) approach yields CsPbBr3 pQDs showing state-of-the-art optical properties at the scale of single emitters. By combining an amine-mediated post-synthetic size-trimming strategy with didodecyldimethylammonium bromide (DDAB) ligands for enhanced surface passivation and colloidal stability, we obtain isolated pQDs with stable emission and minimal spectral diffusion at cryogenic temperatures. Micro-photoluminescence experiments resolve the characteristic fine structure of the bright exciton, its low-energy optical phonon replicas, and the trion and biexciton states. Time-resolved and photon correlation measurements show a ~90 ps lifetime and high purity single photon emission, respectively. These results demonstrate that modified LARP synthesis constitutes an accessible alternative to hot injection, preserving the intrinsic excitonic and quantum optical properties of individual pQDs while offering greater flexibility for post-synthetic ligand engineering, as exemplified here by the use of DDAB for surface passivation.