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Hong–Ou–Mandel interference in colloidal CsPbBr3 perovskite nanocrystals

Nature Photonics volume 17, pages 775–780 (2023)Cite this article

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Abstract

In the search for novel, robust quantum emitters, inorganic lead halide perovskite nanocrystals have emerged as potential colloidal sources of coherent single photons. While colloidal perovskite nanocrystals offer a great source of synthetically scalable, tunable photon sources, observation of two-photon quantum interference from the emission of any colloidal nanoparticle has not been previously reported. In this work we prepare large CsPbBr3 nanocrystals and observe direct evidence of interference between indistinguishable single photons sequentially emitted from a single nanocrystal. We measure Hong–Ou–Mandel interference from photons in CsPbBr3 nanocrystals, showing corrected visibilities of up to 0.56 ± 0.12 in the absence of any radiative enhancement or photonic architecture. These results demonstrate the unique potential of perovskite nanocrystals to serve as scalable, colloidal sources of indistinguishable single photons.

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Fig. 1: Room-temperature ensemble spectra and HAADF-STEM images of PNCs in this work.
Fig. 2: Photoluminescence, time trace and polarization data.
Fig. 3: Hong–Ou–Mandel interferometry and biexciton filtering.
Fig. 4: Coalescence of indistinguishable photons revealed by correlation functions.

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Data availability

All the datasets that support the findings of this study are available on Figshare or from the corresponding author on reasonable request. Source Data are provided with this paper.

References

  1. Knill, E., Laflamme, R. & Milburn, G. J. A scheme for efficient quantum computation with linear optics. Nature 409, 46–52 (2001).

    Article  ADS  Google Scholar 

  2. Tanzilli, S. et al. A photonic quantum information interface. Nature 437, 116–120 (2005).

    Article  ADS  Google Scholar 

  3. O’Brien, J. L., Pryde, G. J., White, A. G., Ralph, T. C. & Branning, D. Demonstration of an all-optical quantum controlled-NOT gate. Nature 426, 264–267 (2003).

    Article  ADS  Google Scholar 

  4. O’Brien, J. L., Furusawa, A. & Vučković, J. Photonic quantum technologies. Nat. Photon. 3, 687–695 (2009).

    Article  ADS  Google Scholar 

  5. Gisin, N., Goire Ribordy, G., Tittel, W. & Zbinden, H. Quantum cryptography. Rev. Mod. Phys. 74, 145 (2002).

  6. Zhang, L., Silberhorn, C. & Walmsley, I. A. Secure quantum key distribution using continuous variables of single photons. Phys. Rev. Lett. 100, 110504 (2008).

  7. Hong, C. K., Ou, Z. Y. & Mandel, L. Measurement of subpicosecond time intervals between two photons by interference. Phys. Rev. Lett. 59, 2044 (1987).

  8. Close, T., Gauger, E. M. & Lovett, B. W. Overcoming phonon-induced dephasing for indistinguishable photon sources. New J. Phys. 14, 113004 (2012).

  9. Reigue, A. et al. Probing electron–phonon interaction through two-photon interference in resonantly driven semiconductor quantum dots. Phys. Rev. Lett. 118, 233602 (2017).

  10. Thoma, A. et al. Exploring dephasing of a solid-state quantum emitter via time- and temperature-dependent Hong–Ou–Mandel experiments. Phys. Rev. Lett. 116, 1–5 (2016).

    Article  Google Scholar 

  11. He, Y. M. et al. On-demand semiconductor single-photon source with near-unity indistinguishability. Nat. Nanotechnol. 8, 213–217 (2013).

    Article  ADS  Google Scholar 

  12. Somaschi, N. et al. Near-optimal single-photon sources in the solid state. Nat. Photon. 10, 340–345 (2016).

    Article  ADS  Google Scholar 

  13. Wang, H. et al. On-demand semiconductor source of entangled photons which simultaneously has high fidelity, efficiency, and indistinguishability. Phys. Rev. Lett. 122, 113602 (2019).

  14. Tomm, N. et al. A bright and fast source of coherent single photons. Nat. Nanotechnol. 16, 399–403 (2021).

    Article  ADS  Google Scholar 

  15. Santori, C. et al. Nanophotonics for quantum optics using nitrogen-vacancy centers in diamond. Nanotechnology 21, 274008 (2010).

  16. Sipahigil, A. et al. Indistinguishable photons from separated silicon-vacancy centers in diamond. Phys. Rev. Lett. 113, 113602 (2014).

  17. Evans, R. E. et al. Photon-mediated interactions between quantum emitters in a diamond nanocavity. Science 362, 662–665 (2018).

    Article  ADS  Google Scholar 

  18. Luo, Y. et al. Carbon nanotube color centers in plasmonic nanocavities: a path to photon indistinguishability at telecom bands. Nano Lett. 19, 9037–9044 (2019).

    Article  ADS  Google Scholar 

  19. Grosso, G. et al. Tunable and high-purity room temperature single-photon emission from atomic defects in hexagonal boron nitride. Nat. Commun. 8, 705 (2017).

  20. Spokoyny, B. et al. Effect of spectral diffusion on the coherence properties of a single quantum emitter in hexagonal boron nitride. J. Phys. Chem. Lett. 11, 1330–1335 (2020).

  21. de Mello Donegá, C., Bode, M. & Meijerink, A. Size- and temperature-dependence of exciton lifetimes in CdSe quantum dots. Phys. Rev. B 74, 085320 (2006).

  22. Utzat, H. et al. Coherent single-photon emission from colloidal lead halide perovskite quantum dots. Science 363, 1068–1072 (2019).

    Article  ADS  Google Scholar 

  23. Beyler, A. P., Marshall, L. F., Cui, J., Brokmann, X. & Bawendi, M. G. Direct observation of rapid discrete spectral dynamics in single colloidal CdSe-CdS core-shell quantum dots. Phys. Rev. Lett. 111, 177401 (2013).

  24. Protesescu, L. et al. Nanocrystals of cesium lead halide perovskites (CsPbX3, X = Cl, Br, and I): novel optoelectronic materials showing bright emission with wide color gamut. Nano Lett. 15, 3692–3696 (2015).

    Article  ADS  Google Scholar 

  25. Kovalenko, M. V., Protesescu, L. & Bodnarchuk, M. I. Properties and potential optoelectronic applications of lead halide perovskite nanocrystals. Science 358, 745–750 (2017).

    Article  ADS  Google Scholar 

  26. Zhang, F. et al. Brightly luminescent and color-tunable colloidal CH3NH3PbX3 (X = Br, I, Cl) quantum dots: potential alternatives for display technology. ACS Nano 9, 4533–4542 (2015).

    Article  Google Scholar 

  27. Tong, Y. et al. From precursor powders to CsPbX3 perovskite nanowires: one-pot synthesis, growth mechanism, and oriented self-assembly. Angew. Chem. Int. Ed. 56, 13887–13892 (2017).

    Article  ADS  Google Scholar 

  28. Krieg, F. et al. Colloidal CsPbX3 (X = Cl, Br, I) nanocrystals 2.0: Zwitterionic capping ligands for improved durability and stability. ACS Energy Lett. 3, 641–646 (2018).

    Article  Google Scholar 

  29. Becker, M. A. et al. Bright triplet excitons in caesium lead halide perovskites. Nature 553, 189–193 (2018).

    Article  ADS  Google Scholar 

  30. Utzat, H. et al. Probing linewidths and biexciton quantum yields of single cesium lead halide nanocrystals in solution. Nano Lett. 17, 6838–6846 (2017).

    Article  ADS  Google Scholar 

  31. Sercel, P. C. et al. Exciton fine structure in perovskite nanocrystals. Nano Lett. 19, 4068–4077 (2019).

    Article  ADS  Google Scholar 

  32. Empedocles, S. A. & Bawendi, M. G. Influence of spectral diffusion on the line shapes of single CdSe nanocrystallite quantum dots. J. Phys. Chem. B 103, 1826–1830 (1999).

    Article  Google Scholar 

  33. Santori, C., Fattal, D., Vučković, J., Solomon, G. S. & Yamamoto, Y. Indistinguishable photons from a single-photon device. Nature 419, 594–597 (2002).

    Article  ADS  Google Scholar 

  34. Schöll, E. et al. Resonance fluorescence of GaAs quantum dots with near-unity photon indistinguishability. Nano Lett. 19, 2404–2410 (2019).

    Article  ADS  Google Scholar 

  35. Madsen, K. H. et al. Efficient out-coupling of high-purity single photons from a coherent quantum dot in a photonic-crystal cavity. Phys. Rev. B 90, 155303 (2014).

  36. Yan, J. et al. Double-pulse generation of indistinguishable single photons with optically controlled polarization. Nano Lett. 22, 1483–1490 (2022).

    Article  ADS  Google Scholar 

  37. Dusanowski, Ł. et al. Purcell-enhanced and indistinguishable single-photon generation from quantum dots coupled to on-chip integrated ring resonators. Nano Lett. 20, 6357–6363 (2020).

    Article  ADS  Google Scholar 

  38. Bylander, J., Robert-Philip, I. & Abram, I. Interference and correlation of two independent photons. European Phys. J. D 22, 295–301 (2003).

    Article  ADS  Google Scholar 

  39. Huber, T., Predojević, A., Föger, D., Solomon, G. & Weihs, G. Optimal excitation conditions for indistinguishable photons from quantum dots. New J. Phys. 17, 123025 (2015).

  40. Reindl, M. et al. Phonon-assisted two-photon interference from remote quantum emitters. Nano Lett. 17, 4090–4095 (2017).

    Article  ADS  Google Scholar 

  41. Hudson, A. J. et al. Coherence of an entangled exciton-photon state. Phys. Rev. Lett. 99, 266802 (2007).

    Article  ADS  Google Scholar 

  42. Muller, A., Fang, W., Lawall, J. & Solomon, G. S. Creating polarization-entangled photon pairs from a semiconductor quantum dot using the optical stark effect. Phys. Rev. Lett. 103, 217402 (2009).

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Acknowledgements

A.E.K.K, C.J.K., W.S., T.S. and D.B.B. acknowledge support from the US Department of Energy, Office of Basic Energy Sciences, Division of Materials Sciences and Engineering under award no. DE-SC00216. H.U. acknowledges support from the US Department of Energy, Office of Basic Energy Sciences, Division of Materials Sciences and Engineering (under award no. DE-FG02-07ER46454). T.S. also acknowledges support from Graduate Fellowship from the Natural Sciences and Engineering Research Council of Canada (NSERC). A.H.P. acknowledges support from a post-doctoral fellowship from the Natural Sciences and Engineering Research Council of Canada (NSERC). C.J.K. thanks A. Penn at MIT.nano for assistance with HAADF-STEM measurements, which were performed in part through the use of MIT.nano’s facilities.

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  1. Hendrik Utzat

    Present address: College of Chemistry, University of California, Berkeley, Berkeley, CA, USA

Authors and Affiliations

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

    Alexander E. K. Kaplan, Chantalle J. Krajewska, Andrew H. Proppe, Weiwei Sun, Tara Sverko, David B. Berkinsky, Hendrik Utzat & Moungi G. Bawendi

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Contributions

A.E.K.K. and H.U. conceived of the study. A.E.K.K. designed the experiment, performed sample preparation, acquired all of the single-nanocrystal data and performed all of the data analysis. C.J.K. synthesized the CsPbBr3 perovskite nanocrystals and acquired all of the ensemble data. A.H.P. aided the background research and data interpretation. W.S. assisted in designing the optical set-up and in developing sample preparation procedures. T.S. and D.B.B. helped develop sample preparation procedures. A.E.K.K. wrote the manuscript and all of the authors provided feedback and comments. M.G.B. directed and supervised the research.

Corresponding author

Correspondence to Moungi G. Bawendi.

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Nature Photonics thanks the anonymous reviewers for their contribution to the peer review of this work.

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Supplementary Discussion and Figs. 1–8.

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Kaplan, A.E.K., Krajewska, C.J., Proppe, A.H. et al. Hong–Ou–Mandel interference in colloidal CsPbBr3 perovskite nanocrystals. Nat. Photon. 17, 775–780 (2023). https://doi.org/10.1038/s41566-023-01225-w

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