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Highly stable and pure single-photon emission with 250 ps optical coherence times in InP colloidal quantum dots

Nature Nanotechnology volume 18, pages 993–999 (2023)Cite this article

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Abstract

Quantum photonic technologies such as quantum communication, sensing or computation require efficient, stable and pure single-photon sources. Epitaxial quantum dots (QDs) have been made capable of on-demand photon generation with high purity, indistinguishability and brightness, although they require precise fabrication and face challenges in scalability. By contrast, colloidal QDs are batch synthesized in solution but typically have broader linewidths, low single-photon purities and unstable emission. Here we demonstrate spectrally stable, pure and narrow-linewidth single-photon emission from InP/ZnSe/ZnS colloidal QDs. Using photon correlation Fourier spectroscopy, we observe single-dot linewidths as narrow as ~5 µeV at 4 K, giving a lower-bounded optical coherence time, T2, of ~250 ps. These dots exhibit minimal spectral diffusion on timescales of microseconds to minutes, and narrow linewidths are maintained on timescales up to 50 ms, orders of magnitude longer than other colloidal systems. Moreover, these InP/ZnSe/ZnS dots have single-photon purities g(2)(τ = 0) of 0.077–0.086 in the absence of spectral filtering. This work demonstrates the potential of heavy-metal-free InP-based QDs as spectrally stable sources of single photons.

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Fig. 1: InP/ZnSe/ZnS QD structure and energy levels.
Fig. 2: Tracking spectral stability on a timescale of seconds–minutes.
Fig. 3: Using PCFS to track spectral diffusion on microsecond–millisecond timescales.
Fig. 4: Γ extracted from interferogram fits at different τ for dots InP-1–3 and CdSe-1.
Fig. 5: Single-photon emission properties of colloidal InP/ZnSe/ZnS QDs.

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Data availability

The data that support the plots within this paper and other findings of this study are available via Zenodo at https://doi.org/10.5281/zenodo.7884365. The data that support the findings of this study are also available from the corresponding author upon reasonable request.

Code availability

All code and scripts used in this study are available from the corresponding author upon reasonable request. For analysing the PCFS experiments, code and examples are available at https://github.com/nanocluster/photons.

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Acknowledgements

A.H.P., D.B.B., T.Š., A.E.K.K. and J.R.H. were supported by the Samsung Advanced Institute of Technology (SAIT). H.Z. was supported by the National Science Foundation (Award No. CHE-2108357). A.H.P. was also supported by a Postdoctoral Fellowship from the Natural Sciences and Engineering Research Council of Canada (NSERC). This work was supported by SAIT, Samsung Electronics Co., Ltd.

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  1. These authors contributed equally: Andrew H. Proppe, David B. Berkinsky.

Authors and Affiliations

  1. Department of Chemistry, Massachusetts Institute of Technology, Cambridge, MA, USA

    Andrew H. Proppe, David B. Berkinsky, Hua Zhu, Tara Šverko, Alexander E. K. Kaplan, Jonah R. Horowitz & Moungi G. Bawendi

  2. Samsung Advanced Institute of Technology, Samsung Electronics, Suwon-si, Republic of Korea

    Taehyung Kim, Heejae Chung & Shinae Jun

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Contributions

A.H.P. and D.B.B. contributed equally to this work. A.H.P. acquired all experimental data and performed all data fitting and analysis. D.B.B. assisted in acquiring all experimental data and data analysis. T.Š. assisted with sample preparation and the optical setup. A.E.K.K. assisted with the optical setup. J.R.H. assisted with data collection of the QD radiative lifetimes. H.Z. provided the CdSe/CdS/ZnS QDs and their TEM images. T.K. and H.C. provided the InP/ZnSe/ZnS dots and their TEM images. M.G.B. and S.J. supervised the project. All authors read and commented on the manuscript.

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Correspondence to Moungi G. Bawendi.

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Proppe, A.H., Berkinsky, D.B., Zhu, H. et al. Highly stable and pure single-photon emission with 250 ps optical coherence times in InP colloidal quantum dots. Nat. Nanotechnol. 18, 993–999 (2023). https://doi.org/10.1038/s41565-023-01432-0

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