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Solution-phase sample-averaged single-particle spectroscopy of quantum emitters with femtosecond resolution

Nature Materials (2024)Cite this article

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Abstract

The development of many quantum optical technologies depends on the availability of single quantum emitters with near-perfect coherence. Systematic improvement is limited by a lack of understanding of the microscopic energy flow at the single-emitter level and ultrafast timescales. Here we utilize a combination of fluorescence correlation spectroscopy and ultrafast spectroscopy to capture the sample-averaged dynamics of defects with single-particle sensitivity. We employ this approach to study heterogeneous emitters in two-dimensional hexagonal boron nitride. From milliseconds to nanoseconds, the translational, shelving, rotational and antibunching features are disentangled in time, which quantifies the normalized two-photon emission quantum yield. Leveraging the femtosecond resolution of this technique, we visualize electron–phonon coupling and discover the acceleration of polaronic formation on multi-electron excitation. Corroborated with theory, this translates to the photon fidelity characterization of cascaded emission efficiency and decoherence time. Our work provides a framework for ultrafast spectroscopy in heterogeneous emitters, opening new avenues of extreme-scale characterization for quantum applications.

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Fig. 1: Experimental scheme and FCS measurements at μs–ms timescales.
Fig. 2: FCS measurements at ns–ms timescales at varying conditions.
Fig. 3: SA-SPPP setup and spectrally resolved photon correlation analysis.
Fig. 4: SA-SPPP measurements on hBN SQEs and polaron simulation.

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Data availability

The data that support the findings of this study are available from the corresponding author upon request.

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Acknowledgements

This work is primarily supported by the US Department of Energy, Office of Science, National Quantum Information Science Research Centers. Y.S. acknowledges support from the Department of Energy, Office of Science, Basic Energy Sciences, Materials Sciences and Engineering Division, under contract DE-AC02-76SF00515 for the polaron simulations. F.P. and J.A.D. acknowledge support from the US Department of Energy, Office of Basic Energy Sciences (award DE-SC0021984), and the Office of Naval Research under the Multi-University Research Initiative (MURI) program (award N00014-23-1-2567) for FCS characterization and modeling efforts. Work was performed in part at the Stanford Nanofabrication Facility supported by the National Science Foundation as part of the National Nanotechnology Coordinated Infrastructure (award ECCS-1542152). W.S. and M.G.B. acknowledge support from the US Department of Energy, Office of Basic Energy Sciences, Division of Materials Sciences and Engineering (award DE-SC0021650). This material is based on the work supported by the US Department of Energy, Office of Science, National Quantum Information Science Research Centers. We also acknowledge helpful discussions with H. Utzat and W. Carpenter.

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Author notes

  1. These authors contributed equally: Jiaojian Shi, Yuejun Shen, Feng Pan.

Authors and Affiliations

  1. Department of Materials Science and Engineering, Stanford University, Stanford, CA, USA

    Jiaojian Shi, Yuejun Shen, Feng Pan, Anudeep Mangu, Cindy Shi, Parivash Moradifar, Jennifer A. Dionne & Aaron M. Lindenberg

  2. Stanford Institute for Materials and Energy Sciences, SLAC National Accelerator Laboratory, Menlo Park, CA, USA

    Jiaojian Shi, Yuejun Shen, Anudeep Mangu & Aaron M. Lindenberg

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

    Weiwei Sun & Moungi G. Bawendi

  4. Department of Chemistry, Stanford University, Stanford, CA, USA

    Amy McKeown-Green, W. E. Moerner & Fang Liu

  5. Department of Radiology, Stanford University, Stanford, CA, USA

    Jennifer A. Dionne

  6. Stanford PULSE Institute, SLAC National Accelerator Laboratory, Menlo Park, CA, USA

    Aaron M. Lindenberg

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Contributions

J.S. and A.M.L. conceived the study. J.S., Y.S. and F.P. conducted the experiment under the supervision of A.M.L., F.L. and J.A.D. F.P. and J.S. interpreted the FCS data under the guidance of W.E.M. Y.S. and J.S. performed the polaronic simulation under the guidance of A.M.L. W.S. provided the CdSe/CdS QDs under the supervision of M.G.B. C.S. prepared the diluted QD solution. C.S. and P.M. performed the transmission electron microscopy characterization. W.S., A.M. and A.M.-G. contributed to data interpretation. J.S., Y.S. and F.P. wrote the paper with crucial inputs from all authors.

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Correspondence to Aaron M. Lindenberg.

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Shi, J., Shen, Y., Pan, F. et al. Solution-phase sample-averaged single-particle spectroscopy of quantum emitters with femtosecond resolution. Nat. Mater. (2024). https://doi.org/10.1038/s41563-024-01855-7

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