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arXiv:quant-ph/9909059 · Physical Review A

Quantum interference in the fluorescence of a molecular system

Jin Wang, Howard M. Wiseman, Z. Ficek

Published Jun 16, 2000• 27 citations
arXivHTMLPDF

Abstract

It has been observed experimentally [H.R. Xia, C.Y. Ye, and S.Y. Zhu, Phys. Rev. Lett. 77, 1032 (1996)] that quantum interference between two molecular transitions can lead to a suppression or enhancement of spontaneous emission. This is manifest in the fluorescent intensity as a function of the detuning of the driving field from the two-photon resonance condition. Here we present a theory that explains the observed variation of the number of peaks with the mutual polarization of the molecular transition dipole moments. Using master equation techniques we calculate analytically as well as numerically the steady-state fluorescence, and find that the number of peaks depends on the excitation process. If the molecule is driven to the upper levels by a two-photon process, the fluorescent intensity consists of two peaks regardless of the mutual polarization of the transition dipole moments. If the excitation process is composed of both a two-step, one-photon process and a one-step, two-photon process, then there are two peaks on transitions with parallel dipole moments and three peaks on transitions with antiparallel dipole moments. This latter case is in excellent agreement with the experiment.

DOI
10.1103/physreva.62.013818

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It has been observed experimentally [H.R. Xia, C.Y. Ye, and S.Y. Zhu, Phys. Rev. Lett. 77, 1032 (1996)] that quantum interference between two molecular transitions can lead to a suppression or enhancement of spontaneous emission. This is manifest in the fluorescent intensity as a function of the detuning of the driving field from the two-photon resonance condition. Here we present a theory that explains the observed variation of the number of peaks with the mutual polarization of the molecular transition dipole moments. Using master equation techniques we calculate analytically as well as numerically the steady-state fluorescence, and find that the number of peaks depends on the excitation process. If the molecule is driven to the upper levels by a two-photon process, the fluorescent intensity consists of two peaks regardless of the mutual polarization of the transition dipole moments. If the excitation process is composed of both a two-step, one-photon process and a one-step, two-photon process, then there are two peaks on transitions with parallel dipole moments and three peaks on transitions with antiparallel dipole moments. This latter case is in excellent agreement with the experiment.
The resonance fluorescence from a four-level atom driven by two coherent fields is studied. If the dipole moments between the two upper levels and each of the two lower levels are parallel, the spontaneous emission paths from the upper levels to the lower levels will have strongly or even completely destructive quantum interference. We show that this quantum interference will result in a complete inhibition of the fluorescence when one of the driving fields is tuned at the middle point of the upper levels. The quantum interference will lead to the dependence of atomic populations at steady state on the initial condition, when both of the driving fields are tuned to the middle point of the upper levels. When the dipole moments are close to but not exactly parallel, or none of the driving fields is tuned at the middle point of the upper levels and there is a small difference between detunings of the two driving fields to the uppermost level, ultranarrow lines at the spectral center appear because of the destructive quantum interference.
In this review the author discusses the major effects resulting from the modification of spontaneous emission by quantum interference. He begins in Section II by presenting elementary concepts and definitions of the first- and second-order correlation functions, which are frequently used in the analysis of the interference phenomena. Section III describes the master equation approach used for analyzing quantum interference effects in atomic and molecular systems. In Sections IV and V the author reviews the fundamental quentum interference effects in spontaneous emission and in coherently driven systems. He discusses different schemes for suppression of spontaneous emission and population trapping and gives an alternative explanation of these effects in the dressed-atom picture. Section VI deals with the problem of amplification on dark transitions, which are important for information processing without spontaneous emission. The effect of quantum interference on photon correlations is discussed in Section VII. Multilevel systems composed of two transitions with parallel dipole moments and methods for generating two transitions with nonorthogonal dipole moments are briefly discussed in Section VIII. The final section (Section IX) deals with the experimental demonstration of constructive and desctructive interference effects in a driven molecular system.
We show that a dynamical suppression of spontaneous emission, predicted for a three-level atom [S.-Y. Zhu and M. O. Scully, Phys. Rev. Lett. 76, 388 (1996)] can occur in a two-level atom driven by a polychromatic field. We find that the quantum interference, responsible for the cancellation of spontaneous emission, appears between different channels of transitions among the dressed states of the driven atom. We discuss the effect for bichromatic and trichromatic (amplitude-modulated) fields and find that these two cases lead to the cancellation of spontaneous emission in different parts of the fluorescence spectrum. Our system has the advantage of being easily accessible by current experiments.
In a recent experiment by Eichmann et al. [Phys. Rev. Lett. 70, 2359 (1993)], polarization-sensitive measurements of the fluorescence from two four-level ions driven by a linearly polarized laser were made. Depending on the polarization chosen, different degrees of interference were observed. We carry out a theoretical and numerical study of this system, showing that the results can largely be understood by treating the atoms as independent radiators which are synchronized by the phase of the incident laser field. The interference and its loss may be described in terms of the difference between coherent and incoherent driving of the various atomic transitions in the steady state. In the numerical simulations, which are carried out using the Monte Carlo wave-function method, we remove the assumption that the atoms radiate independently and consider the photodetection process in detail. This allows us to see the total interference pattern build up from individual photodetections and also to see the effects of superfluorescence, which become important when the atomic separation is comparable to an optical wavelength. The results of the calculations are compared with the experiment. We also carry out simulations in the non-steady-state regime and discuss the relationship between the visibility of the interference pattern and which-path considerations.
The interference spectra arising from the competition between a spontaneous process and an induced one by two laser fields, which interact on two-photon resonance with a three-level atom in the Lambda configuration have been considered. In the low intensity limit of both laser fields, the frequency profiles of the two peaks, which arise from the spontaneous and induced processes, respectively, cancel each other out completely at the centre of the line for zero detuning and at the finite values of the detuning as well. At those frequencies, the fluorescent light totally disappears. The interference spectra arising from the absorption of a laser photon by the ground state of the atom consists of two peaks describing the induced processes of absorption and stimulated emission, respectively.
It is shown that when a monochromatic laser couples a single atomic ground level to two closely spaced excited levels the system can be driven into a state in which quantum interference prevents any fluorescence from the excited levels, regardless of the intensity of the exciting field. This steady-state interference occurs only at a particular excitation frequency which depends on the separation of the excited states and the relative size of the two transition dipole matrix elements. The results are derived from the density matrix equations of motion. It is shown that a correct description of the effect requires the inclusion of generalised Einstein A coefficients which are usually neglected in phenomenological damping theories. A dressed-state analysis is introduced to simplify the generalisation to atoms having more complex manifolds of excited states. Analogous interferences in multiphoton absorption and ionisation are also discussed briefly.