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Super- and sub-Poissonian photon statistics for single molecule spectroscopy
1Department of Chemistry and Biochemistry, Notre Dame University, Notre Dame, Indiana 46556, USA.
The Journal of Chemical Physics
|May 28, 2005
Summary
This study reveals how spectral diffusion affects photon emission from single molecules. We found Mandel's Q parameter transitions from quantum sub-Poissonian to classical super-Poissonian behavior based on modulation speed.
Area of Science:
- Quantum Optics
- Spectroscopy
- Statistical Physics
Background:
- Spectral diffusion significantly impacts light-matter interactions in single molecules.
- Understanding photon statistics is crucial for quantum information and sensing.
Purpose of the Study:
- To analytically determine the photon emission distribution and Mandel's Q parameter for a single molecule with spectral diffusion under continuous wave laser excitation.
- To investigate the influence of spectral diffusion dynamics and laser field strength on photon statistics.
Main Methods:
- Stochastic modeling of spectral diffusion based on Anderson-Kubo line shape theory.
- Generating function formalism to solve generalized optical Bloch equations.
- Derivation of exact analytical formulas for line shape and Mandel's Q parameter.
Main Results:
- The line shape shows motional narrowing and power broadening.
- Mandel's Q parameter exhibits a transition from sub-Poissonian (fast modulation) to super-Poissonian (slow modulation) behavior.
- Analytical results are valid for weak and strong laser fields (arbitrary Rabi frequency).
Conclusions:
- The study provides a comprehensive theoretical framework for photon statistics in spectrally diffusing systems.
- Optimal Rabi frequencies can enhance the quantum sub-Poissonian nature of emission.
- Non-trivial behavior emerges in intermediate modulation regimes, bridging quantum and classical descriptions.
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