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Solution-phase sample-averaged single-particle spectroscopy of quantum emitters with femtosecond resolution.
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.
Afiliação
  • Shi J; Department of Materials Science and Engineering, Stanford University, Stanford, CA, USA.
  • Shen Y; Stanford Institute for Materials and Energy Sciences, SLAC National Accelerator Laboratory, Menlo Park, CA, USA.
  • Pan F; Department of Materials Science and Engineering, Stanford University, Stanford, CA, USA.
  • Sun W; Stanford Institute for Materials and Energy Sciences, SLAC National Accelerator Laboratory, Menlo Park, CA, USA.
  • Mangu A; Department of Materials Science and Engineering, Stanford University, Stanford, CA, USA.
  • Shi C; Department of Chemistry, Massachusetts Institute of Technology, Cambridge, MA, USA.
  • McKeown-Green A; Department of Materials Science and Engineering, Stanford University, Stanford, CA, USA.
  • Moradifar P; Stanford Institute for Materials and Energy Sciences, SLAC National Accelerator Laboratory, Menlo Park, CA, USA.
  • Bawendi MG; Department of Materials Science and Engineering, Stanford University, Stanford, CA, USA.
  • Moerner WE; Department of Chemistry, Stanford University, Stanford, CA, USA.
  • Dionne JA; Department of Materials Science and Engineering, Stanford University, Stanford, CA, USA.
  • Liu F; Department of Chemistry, Massachusetts Institute of Technology, Cambridge, MA, USA.
  • Lindenberg AM; Department of Chemistry, Stanford University, Stanford, CA, USA.
Nat Mater ; 23(8): 1063-1069, 2024 Aug.
Article em En | MEDLINE | ID: mdl-38589542
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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Texto completo: 1 Coleções: 01-internacional Base de dados: MEDLINE Idioma: En Revista: Nat Mater Assunto da revista: CIENCIA / QUIMICA Ano de publicação: 2024 Tipo de documento: Article País de afiliação: Estados Unidos
Texto completo
Imprimir
XML
PubMed Links
Buscar no Google

Texto completo: 1 Coleções: 01-internacional Base de dados: MEDLINE Idioma: En Revista: Nat Mater Assunto da revista: CIENCIA / QUIMICA Ano de publicação: 2024 Tipo de documento: Article País de afiliação: Estados Unidos