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Physical Review A

Mode coupling in a vibronic laser

F. Marquis, P. Schwendimann

Published Jan 1, 1989• 3 citations
Publisher

Abstract

Taking into account the vibronic-level structure in a laser medium, we study the influence of electron-vibration interaction on the field dynamics. Different vibronic transitions are coupled in the medium through this interaction and contribute to the emission from excited states, thus coupling different field modes in the cavity and influencing the field dynamics. A general model is presented and solved in a simple example of four coupled transitions. In particular, the effect of degenerate transitions is stressed.

DOI
10.1103/physreva.39.157

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Herewith we present the quantum theory of the vibronic laser, which is based on the crucial role played by the host crystal phonons in the laser dynamics. In the solid state transition-metal ion laser the operation takes place between the vibronically broadened electronic levels of the gain center, thus the laser action is accompanied by the creation or annihilation of the host lattice phonons. The nonequilibrium coherent phonons, produced in the process of the nonradiative energy transition from the photoexcited impurity ion, pump the energy level, from whivh the laser action takes place. One can say that the laser photons are produced at the cost of lattice phonons. This is the reason why the coherent phonons strongly influence the character of the laser action and govern the complicated laser dynamics. In the laser equations, derived by us, the number of coherent phonons is treated as one of dynamical variables coupled with the number of photons. In solution we observe the eect of energy pulling between photons and phonons. Phonons follow all forms of the photon dynamics including self-pulsations and chaotic dynamics.

•Jan 1, 2008•0 citations
Taking into account the vibronic-level structure in a laser medium, we study the influence of electron-vibration interaction on the field dynamics. Different vibronic transitions are coupled in the medium through this interaction and contribute to the emission from excited states, thus coupling different field modes in the cavity and influencing the field dynamics. A general model is presented and solved in a simple example of four coupled transitions. In particular, the effect of degenerate transitions is stressed.
The resonance fluorescence from a vibronic system with displaced potential-energy surfaces is studied. Because of the equal vibrational frequencies in the two electronic quantum states, a large number of vibronic transitions can be excited by a strong laser field. Even in the case of weaker driving fields, nonperturbative effects may be observed provided that the vibrational relaxation is slow enough. If the vibronic coupling is not extremely strong, the Rabi oscillations will arise mainly from the excitation of the vibrationless transition. Furthermore, the damping of the Rabi oscillations may be accompanied by a substantial decrease in intensity.
The problem of resonant interaction between an electromagnetic radiation field and a vibronic system, such as a molecule or a localized electronphonon system, is considered. The vibronic coupling is assumed to result from displaced and distorted potential energy surfaces for the vibrational motion in the electronic quantum states involved in the resonant interaction with the radiation field. Furthermore, the vibrational energy relaxation is taken into account without assumptions about Markovian-type relaxation. In order to study correlation properties of higher than second order in the electric field strength of the light emitted a method of calculation of the expectation value of an arbitrary product combination of effective time evolution operators of the vibronic system is developed. The calculations are performed by utilizing Feynman's disentangling and operator ordering techniques and yield closed solutions in the low-temperature limit. The theory is used for studying the intensity and the normally ordered intensity correlation function of the resonance fluorescence light from a two-atom molecule excited by a relatively weak laser field, which undergoes phase fluctuations. It is shown that the vibronic coupling can give rise to an anticorrelation effect which is substantially stronger than in the case of resonance fluorescence from an atom. For the case of small vibrational damping a general formula which directly connects the asymptotic long-time behaviour of the normalized intensity correlation function with the vibrational relaxation in the molecule is deduced. It should be convenient for the determination of very small vibrational decay rates.
The stationary second-order spectrum of the resonance-fluorescence light from a vibronic system is studied in a nonperturbative manner. In the model used the potential energy surfaces for the vibrational motion in the electronic ground state and in the excited state are assumed to be displaced and distorted relative to each other. The calculations are performed for the case when the frequency of the driving laser field is tuned to the vibrationless electronic transition. In particular, in the high-driving-field limit the vibrationless transition exhibits a triplet structure, the sidebands being narrower and higher in comparison with the well-known two-level case. The Raman lines are shifted and split into doublets, the linewidths being determined by the electronic as well as the vibrational relaxation rates.
Herewith we present the quantum theory of the vibronic laser, which is based on the crucial role played by the host crystal phonons in the laser dynamics. In the solid state transition-metal ion laser the operation takes place between the vibronically broadened electronic levels of the gain center, thus the laser action is accompanied by the creation or annihilation of the host lattice phonons. The nonequilibrium coherent phonons, produced in the process of the nonradiative energy transition from the photoexcited impurity ion, pump the energy level, from whivh the laser action takes place. One can say that the laser photons are produced at the cost of lattice phonons. This is the reason why the coherent phonons strongly influence the character of the laser action and govern the complicated laser dynamics. In the laser equations, derived by us, the number of coherent phonons is treated as one of dynamical variables coupled with the number of photons. In solution we observe the eect of energy pulling between photons and phonons. Phonons follow all forms of the photon dynamics including self-pulsations and chaotic dynamics.