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Physical Review A

Control of the photon emission of single molecules in a solid matrix

Baiping Han, Yujun Zheng

Published Jul 16, 2008• 23 citations
Publisher

Abstract

We consider the photon spontaneous emission of single molecules in a solid matrix with spectral diffusion. A general theoretical strategy for calculating the photon emission statistics in a solid matrix of single molecules is derived. In particular, the control photon emission from single molecules in a solid matrix driven simultaneously by a laser and an electric radiofrequency (rf) field is investigated. The photon emission of single molecules can be modulated by an rf field. The formulation also allows for the study of the average waiting time for the emission event of a single molecule.

DOI
10.1103/physreva.78.015402

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We consider the photon spontaneous emission of single molecules in a solid matrix with spectral diffusion. A general theoretical strategy for calculating the photon emission statistics in a solid matrix of single molecules is derived. In particular, the control photon emission from single molecules in a solid matrix driven simultaneously by a laser and an electric radiofrequency (rf) field is investigated. The photon emission of single molecules can be modulated by an rf field. The formulation also allows for the study of the average waiting time for the emission event of a single molecule.
The photon emission from a single molecule driven simultaneously by a laser and a slow electric radio frequency (rf) field is studied. We use a non-Hermitian Hamiltonian approach which accounts for the radiative decay of a two-level system modeling the single-molecule source. We apply the renormalization group method for differential equations to obtain long time solution of the corresponding Schrodinger equation, which allows us to calculate the average waiting time for the first photon emission. Then, we analyze the conditions for suppression and enhancement of photon emission in this dissipative two-level system. In particular we derive a transcendental equation, which yields the nontrivial rf field control parameters, for which enhancement and suppression of photon emission occurs. For finite values of radiative decay rate an abrupt transition to the state when both situations are indistinguishable is found for certain values of the rf field parameters. Our results are shown to be in agreement with the available experiments [Ch. Brunel et al., Phys. Rev. Lett. 81, 2679 (1998)].
In this paper, we study the influence of time-dependent phase delay on the emission of few photons from a single molecule in a solid matrix. The results demonstrate that a time-dependent phase of the pulses can be used to control the photon emission and strongly affects the spectrum of single molecules. The spectrum of the photon emission probabilities reflects the fast dynamics of the states of the system when the duration of the driven laser pulses is short. Also, it is shown that the coupling between the system and the rf field strongly affects the spectrum of the photon emission probabilities in space.
The photon emission from a single molecule driven simultaneously by a laser and a slow electric radio frequency (rf) field is studied. We use a non-Hermitian Hamiltonian approach which accounts for the radiative decay of a two level system modeling a single molecule source. We apply the renormalization group method for differential equations to obtain long time solution of the corresponding Schrdinger equation, which allows us to calculate the average waiting time for the first photon emission. Then, we analyze the conditions for suppression and enhancement of photon emission in this dissipative two-level system. In particular we derive a transcendental equation, which yields the non-trivial rf field control parameters, for which enhancement and suppression of photon emission occurs. For finite values of radiative decay rate an abrupt transition from the molecule's localization in its ground state to delocalization is found for certain critical values of the rf field parameters. Our results are shown to be in agreement with the available experiments [Ch. Brunel et al, Phys. Rev. Lett. 81, 2679 (1998)].