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

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...

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Bibliographic Details
Published in:Nature materials 2024-08, Vol.23 (8), p.1063-1069
Main Authors: Shi, Jiaojian, Shen, Yuejun, Pan, Feng, Sun, Weiwei, Mangu, Anudeep, Shi, Cindy, McKeown-Green, Amy, Moradifar, Parivash, Bawendi, Moungi G., Moerner, W. E., Dionne, Jennifer A., Liu, Fang, Lindenberg, Aaron M.
Format: Article
Language:English
Subjects:
639/301/357/1018
639/301/930/12
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639/624/400/584
Biomaterials
Boron
Boron nitride
Chemistry and Materials Science
Condensed Matter Physics
Defects
Emissions
Emitters
Emitters (electron)
Energy flow
ENGINEERING
Excitation spectra
Fluid flow
Fluorescence
MATERIALS SCIENCE
Nanotechnology
Optical and Electronic Materials
Photon emission
Photons
Rotational spectra
Sensitivity
Shelving
Spectroscopic analysis
Spectroscopy
Spectrum analysis
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Description
Summary: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. Combining fluorescence correlation spectroscopy and ultrafast spectroscopy, the sample-averaged dynamics of defects are studied with single-particle sensitivity in two-dimensional hexagonal boron nitride heterogeneous emitters.
ISSN:1476-1122
1476-4660
1476-4660
DOI:10.1038/s41563-024-01855-7