Third-order photon correlations extract single-nanocrystal multiexciton properties in solution
Name
oe-33-15-31785.pdf
Description
Published version
Size
2.46 MB
Format
Adobe PDF
Checksum (MD5)
303b817cbb82a4f0960e667cf7e8c721
Author(s)
Horowitz, Jonah R
Berkinsky, David B
Bendekgey, Henry C
Tye, Oliver J
Šverko, Tara
Shulenberger, Katherine E
Bawendi, Moungi G
Date Issued
July 28, 2025
Journal
Optics Express
Publisher
Optica Publishing Group
Citation
Jonah R. Horowitz, David B. Berkinsky, Henry C. Bendekgey, Oliver J. Tye, Tara Šverko, Katherine E. Shulenberger, and Moungi G. Bawendi, "Third-order photon correlations extract single-nanocrystal multiexciton properties in solution," Opt. Express 33, 31785-31800 (2025)
Version
Final published version
Abstract
Colloidal semiconductor nanocrystals are considered promising materials for high-flux optical applications, including lasing, light-emitting diodes, biological imaging, and quantum optics. In high-flux applications, multiexcitons can significantly contribute to emission, influencing its brightness, spectral purity, and kinetics. As a result, understanding and controlling multiexciton emission in colloidal nanocrystal materials is of the utmost importance. In the past, single-nanocrystal photon correlation methods have been applied to understand biexciton and triexciton efficiencies, lifetimes, and spectra. While powerful, such methods suffer from user selection bias and require stable emission from single nanocrystals. To compensate for this shortcoming, second-order correlation methods were developed to extract sample-averaged biexciton properties from a solution of nanocrystals. Until now, however, the analogous third-order solution photon correlation methods remained unexplored. In this work, we present a pair of third-order photon correlation techniques to obtain the sample-averaged single-nanocrystal triexciton quantum yield and lifetime in a solution-phase experiment. These techniques derive from the relationship between the Poisson probability of nanocrystal photon absorption and the intrinsic probability of nanocrystal photon emission. We validate the theoretical background of these techniques by creating a numerical model to simulate the diffusion and emission of many nanocrystals in solution. Our simulations confirm that the average triexciton quantum yield and triexciton lifetime can be extracted from a solution of nanocrystals. These techniques will enable researchers to gain a better understanding of the fundamental multiexciton properties of colloidal nanocrystals.
MIT Department
Massachusetts Institute of Technology. Department of Chemistry
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Article is made available in accordance with the publisher's policy and may be subject to US copyright law. Please refer to the publisher's site for terms of use.
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DOI of Published Version
10.1364/oe.564578
