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Optica Acta International Journal of Optics

Stimulated Inelastic Resonance Fluorescence in an Optically Thick Medium

B. Macke, François Rohart

Published Aug 1, 1981• 4 citations
Publisher

Abstract

A non-resonant stepwise optical wave travelling through an ensemble of two-level systems is shown to be accompanied by a resonant optical pulse which is continuously amplified and shortened during the propagation. The sample excitation promoted by this stimulated light is calculated in the limit where the frequency offset is much larger than the linewidth (including the saturation broadening) and is shown to be much below previous estimations and dramatically affected by the rise time of the driving field.

DOI
10.1080/713820683

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A non-resonant stepwise optical wave travelling through an ensemble of two-level systems is shown to be accompanied by a resonant optical pulse which is continuously amplified and shortened during the propagation. The sample excitation promoted by this stimulated light is calculated in the limit where the frequency offset is much larger than the linewidth (including the saturation broadening) and is shown to be much below previous estimations and dramatically affected by the rise time of the driving field.
The optical density of a resonant medium significantly affects the output signal in time resolved nonlinear optical interactions. The resonant interaction with a medium reshapes any propagating short pulse, and the mutual interaction of several such pulses, as in four-wave mixing, must be treated self-consistently. We present a theoretical framework for the proper handling of the propagation of all pulses, input as well as generated, in the small area limit. For optically thick resonant absorbers, negative time delay signals are observed, and the apparent decay rate of the induced polarization is faster than the rate observed for thin samples. We experimentally measure degenerate four-wave mixing in an atomic medium as an example, and demonstrate the quality of the theoretical model by the excellent fit to measured signals over several orders of magnitude. The improved understanding enables us to provide a simple, but surprisingly accurate, estimate for the apparent decay rate in homogeneously broadened optically thick media: If the absorption is given by \ensuremath{\alpha}, the propagation length is L, and the transverse relaxation time is T2{\mathit{T}}_{2}T2​, the apparent decay rate 2/Ta{\mathit{T}}_{\mathit{a}}Ta​ of a time resolved four-wave mixing signal is given by 2/Ta{\mathit{T}}_{\mathit{a}}Ta​=(2/T2{\mathit{T}}_{2}T2​)(1+\ensuremath{\alpha}L/2).
We consider the nonlinear propagation of an intense short pulse of polarized light through a molecular medium with ground- and excited-state absorption, excited-state emission, and fluorescence from the excited state to the ground state and possibly to a lower-lying excited state. We incorporate the effects of saturation, field-induced alignment, and rotational diffusion of the molecules in the medium. Our approach uses a slowly varying envelope approximation for the light propagation and rate equations for the effective parallel and perpendicular (and higher-multipole) population components of the molecular states. The time dependence of the anisotropy of the fluorescence occurring after preparation of the medium by the intense short pulse is determined. We can treat propagation through an optically nonthin medium wherein the intensity of the pulse decreases while propagating through the medium. An example of a 100-ps pulse propagating through a sample of Rhodamine-6G is presented. We compare our method with others used to describe intense-short-pulse propagation in molecular media.
We consider the propagation of a light pulse in a medium with a single resonance. If the frequency of the pulse is tuned far from resonance and the pulse duration is much shorter than the lifetime of the excited state of the resonant particles in the medium (atoms in a gas, impurity ions in a solid, etc.), the group velocity of the pulse is appreciably reduced. It is shown that the slowing down of the group velocity of the pulse is accompanied with a pulse chirp, which produces a pulse broadening in time. It is proposed to use two samples in sequence with opposite chirps (up chirp and down chirp or vice versa) compensating the pulse broadening. Then the pulse can be delayed with almost no losses, distortion, and broadening. However, there is a maximum distance, beyond which the pulse experiences corruption. Pumping with an auxiliary laser beam can control the delay time of the light pulse in the medium. Conditions to eliminate the contribution of the dephasing processes in the pulse propagation are considered.
The line shapes of saturation spectroscopy in optically thick two-level media are calculated for atomic and molecular transitions. Line narrowing and distortion effects due to propagation are presented. For Doppler-broadened media it is shown that, due to multiphoton processes, the natural linewidth limits the ultimate narrowing that can be reached. Thus, up to ${\ensuremath{\alpha}}_{0}L=20,$ only when the rate-equation approximation is valid subhomogeneous linewidths are expected.
The propagation of a strong coherent "pump" wave traveling through a resonant medium is discussed. The medium is assumed to consist of identical stationary atoms, and the pump-wave frequency is assumed to coincide exactly with the resonance frequency for transitions between a particular pair of atomic states. A previously developed theory of the response of a strongly driven atom to a weak nearly resonant "signal" field is used to deduce the existence of a coupling between any two waves travelling parallel to the pump wave whose (nearly equal) frequencies sum to twice the pump-wave frequency. In the limit of very intense (highly saturating) pump fields, the coupling between the two waves of nearby frequencies leads to amplification of both waves if their frequencies lie within an interval about the pump-wave frequency equal to the Rabi frequency of population inversion. The basic process, which is roughly described by travelling-wave parametric-amplifier equations of motion, consists of the absorption of two pump-field photons followed by their emission at different nearby frequencies, and thus implies a frequency instability of the initially coherent pump wave.
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.