Article ; Online: Solution-phase sample-averaged single-particle spectroscopy of quantum emitters with femtosecond resolution.
2024
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 ... ...
| 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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| Language | English |
| Publishing date | 2024-04-08 |
| Publishing country | England |
| Document type | Journal Article |
| ZDB-ID | 2088679-2 |
| ISSN | 1476-4660 ; 1476-1122 |
| ISSN (online) | 1476-4660 |
| ISSN | 1476-1122 |
| DOI | 10.1038/s41563-024-01855-7 |
| Database | MEDical Literature Analysis and Retrieval System OnLINE |
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