Solution-phase sample-averaged single-particle spectroscopy of quantum emitters with femtosecond resolution
Name
2405188.pdf
Description
Accepted version
Size
6.92 MB
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Checksum (MD5)
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Author(s)
Shi, Jiaojian
Shen, Yuejun
Pan, Feng
Sun, Weiwei
Mangu, Anudeep
Shi, Cindy
McKeown-Green, Amy
Moradifar, Parivash
Bawendi, Moungi G
Moerner, WE
Date Issued
April 8, 2024
Journal
Nature Materials
Publisher
Springer Science and Business Media LLC
Citation
Shi, J., Shen, Y., Pan, F. et al. Solution-phase sample-averaged single-particle spectroscopy of quantum emitters with femtosecond resolution. Nat. Mater. 23, 1063–1069 (2024).
Version
Author's final manuscript
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.
MIT Department
Massachusetts Institute of Technology. Department of Chemistry
Terms of Use
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
10.1038/s41563-024-01855-7
