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Physical Review A

Reduction of single-photon emission from a single-emitter system by intersystem crossing

Yong He, Lin Dai

Published Jan 28, 2014• 2 citations
Publisher

Abstract

We investigate the reduction in the probability of single-photon emission from a single-emitter system caused by intersystem crossing. The physical model is that a single-emitter system with three levels is excited by a square pulse laser, and then a single photon is emitted at a controllable time. We find that the intersystem crossing always reduces the probability of single-photon emission. We obtain quantitative and analytical expressions for the probabilities of zero-, one-, and two-photon emission and Mandel's Q parameter as the function of the intersystem crossing rate under the conditions of finite field strength and finite interaction time with the laser pulse. We discuss the conditions for obtaining the maximal probability of single-photon emission in the presence of intersystem crossing. We find that one can obtain a high probability of single-photon emission from the single-emitter system using square pulse excitation in comparison with continuous wave excitation. Mandel's Q parameter exhibits a transition from a sub-Poissonian behavior to a super-Poissonian behavior due to the influence of intersystem crossing. The calculated Mandel's Q parameter and second-order correlation function of photon emission considering the coherent effect are in better agreement with the experimental data.

DOI
10.1103/physreva.89.013839

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We investigate the reduction in the probability of single-photon emission from a single-emitter system caused by intersystem crossing. The physical model is that a single-emitter system with three levels is excited by a square pulse laser, and then a single photon is emitted at a controllable time. We find that the intersystem crossing always reduces the probability of single-photon emission. We obtain quantitative and analytical expressions for the probabilities of zero-, one-, and two-photon emission and Mandel's Q parameter as the function of the intersystem crossing rate under the conditions of finite field strength and finite interaction time with the laser pulse. We discuss the conditions for obtaining the maximal probability of single-photon emission in the presence of intersystem crossing. We find that one can obtain a high probability of single-photon emission from the single-emitter system using square pulse excitation in comparison with continuous wave excitation. Mandel's Q parameter exhibits a transition from a sub-Poissonian behavior to a super-Poissonian behavior due to the influence of intersystem crossing. The calculated Mandel's Q parameter and second-order correlation function of photon emission considering the coherent effect are in better agreement with the experimental data.
We investigate the theory of a few photons on demand from a single two-level emitter excited by a square laser pulse. Using the generalized optical Bloch equations, we find exact expressions for the probability of generating zero, one, two, and three photons, the average ⟨N⟩⟨N⟩⟨N⟩, and Mandel's QQQ parameter, which exhibit rich physical behaviors. The exact solution is used to design control fields that yield an optimal single- or two-photon source, under the constraints of finite laser-field strength and finite interaction time.
We studied the photon statistics of the driven single molecule under intersystem crossing process which caused the fluorescence blinking via generating function approach.We give an analytical expression of the average emission photons N and the Mandel's Q parameter in long time limit.The results demonstrate that the Mandel's Q parameter has the same behavior as the average emission photons N with respect to the evolution time,both of them linearly increasing with the evolution time increase,when the intersystem crossing process occurred in the single molecule.
We studied the photon statistics of the driven single molecule under intersystem crossing process which caused the fluorescence blinking via generating function approach. We give an analytical expression of the average emission photons <N>and the Mandel's Q parameter in long time limit. The results demonstrate that the Mandel's Q parameter has the same behavior as the average emission photons <N> with respect to the evolution time, both of them linearly increasing with the evolution time increase, when the intersystem crossing process occurred in the single molecule.
We consider the theory of single photon on demand from a two level atom or molecule source. Using optical Bloch equations and the generating function formalism we investigate three approaches to single photon control: (i) the square laser pulse; (ii) the square modulation of absorption frequency; and (iii) the rapid adiabatic following approach investigated in the experiments of Brunel et al., Phys. Rev. Lett., 1999, 83, 2722. We discuss the conditions for obtaining the maximum of the probability of emission of a single photon and a pair of photons, under the constrains of finite field strength and finite interaction time with excitation field. We obtain analytical expression for the probability of emitting zero, one, and two photons for the square pulse, and discuss semi-classical and strongly quantum limiting cases. Numerical results obtained from the generating function formalism are compared with experimental results showing that the two level system approach is suitable for the description of cryogenic temperature single molecules, and that experiments were conducted very close to the optimal conditions.
The statistic characteristics of single photon emission in single semiconductor quantum dot with pulse excitation have been investigated.With rotating-wave approximation,we deduce the dynamics equations including second-order correlation function from the master equations of the populations and discuss the correlation function of photon emission from the exciton combination under different input pulse areas.There will appear an apparant split peak around zero time delay under strong excitation.For short pulse width,the probability of single photon emission p and the efficiency of single photon emission η oscillate as the excitation intensity increases.It is revealed that high efficient single photon emissions can be realized in this system when excited with input pulse area about π and short pulse width.
The influence of vacuum fluctuation and phonon bath on the probability of single photon emission are both considered in the two-level system model theoretically; by using the master equations and generating function method we get the analytical expression of the second-order fluorescence correlation function, probability of single photon emission, and Mandel’s Q parameter. The results manifest that the coupling between the phonon bath and single photon source destroys the superposition state induced by the square laser pulse, the Rabi oscillation damped rapidly with the increasing of temperature. Theoretically, when the structure parameter of arsenide quantum dots α scaled to 0.1 times of the sample, the critical coherence-temperature will rise up to hundreds of Kelvin, which means a step forward to the realization of coherent control of single photon source at room temperature.