Using both a bare-atom and dressed-atom picture of atom-field interactions, we present a theory of the pressure-induced resonances that can arise when four radiation fields interact with a three-level quantum system. The four fields drive two coupled atomic transitions which share a common level, the levels being arranged in a ``ladder'' scheme. As the field frequencies are varied, certain resonant structures in the excitation spectrum of the upper state population appear only in the presence of collisions. The resonant structures result from processes that have been referred to in the past as collisionally aided radiative excitation (CARE) and pressure-induced extra resonances in four-wave mixing (PIER4). We show that both CARE- and PIER4-type resonances have a common origin, which can be linked to conservation of energy. In contrast to conventional PIER4 signals, line shapes calculated in this work result from a ``single atom'' rather than a collective emission. Moreover, the signals vanish unless the applied fields are relatively coherent, again in contrast to conventional PIER4.
Pressure-induced effects in nonlinear optics and spectroscopy are studied using a nonstandard-dressed-atom formalism for a set of two-level atoms. We consider a two-level atom interacting with two radiation fields whose frequencies differ by \ensuremath{\delta} and undergoing dephasing collisions with a perturber bath. The atom-field detunings are large compared with all relaxation rates in the problem. The system is described by a Hamiltonian of an atom dressed by a single-mode field with a coupling constant slowly varying in time at frequency \ensuremath{\delta}. We show that the collisionally aided excitation of the initially unpopulated dressed states is modulated in time. All the characteristics of the pressure-induced effects are deduced from the properties of this time-modulated excitation. Apart from already known phenomena (pressure-induced extra resonances in four-wave mixing, pressure-induced phase shifts, etc.) that are reinterpreted using this approach, we present a new effect that can be described as fluorescence beats. Finally, we show that this approach gives a firm basis for use of a model involving collision-induced gratings and we interpret the pressure-induced effects in the context of this model.
We develop a general dressed-state framework for computing fluorescence spectra, probe absorption spectra, and photon-photon correlations of light scattered by ensembles of
Nat two-level atoms with arbitrary
Jg→Je transitions driven by intense coherent fields. The approach employs a full vectorial treatment of the electromagnetic field, handles any atomic geometries, illumination directions, and polarizations, and yields optical observables as explicit sums of Lorentzian lines whose positions, widths, and weights are directly tied to the eigenvalues and eigenvectors of the Lindbladian. The framework is implemented in an open-source Python package and benchmarked against exact single- and two-atom calculations. We identify geometries in which the full vectorial description is essential, and the scalar approximation fails qualitatively. Applying the method to pairs of atoms with a
Jg=0→Je=1 transition, we show that elastic and inelastic scattered intensities collapse onto universal master curves controlled by a single collective saturation parameter built from the dominant superradiant mode, across several orders of magnitude in drive strength and interatomic distance. We identify collective phenomena that require a description beyond this single-mode picture. Extending the analysis to atoms with ground-state degeneracy, we find that most collective features carry over, while two qualitatively new effects emerge: an incoherent spontaneous Raman channel that modifies the scaling of inelastic emission, and a slow timescale in the time-delayed correlations
g(2)(τ) governed by the competition between Raman scattering and subradiant decay, controlled by a single dimensionless parameter. These results provide both physical insight and practical computational tools for engineering collective optical responses in few-atom systems such as optical tweezer arrays.
The effect of pump fluctuations on various coherent processes that arise in three-level systems interacting with two external fields is examined. Such coherent processes include the forward Hanle effect and various four-wave mixing effects such as the generation of phase-conjugate signals. A general formulation that enables one to calculate the influence of laser linewidth on the coherent signals produced in various directions is presented. Ensemble averages, over laser temporal fluctuations, of various physical quantities, such as atomic polarization, are calculated. The spectrum of polarization fluctuations is shown to consist of several new features which lead to coherent radiation in different directions depending on the resonant frequencies in the polarization fluctuations. The influence of pump linewidth on pressure-induced extra resonance (PIER) is treated in detail. The possibility of producing a laser-fluctuation-induced coherent signal at one of the atomic frequencies is examined. This new signal, which is produced in a direction different from that of the PIER signal, but has the same type of resonant character as PIER, is found to have significantly different pressure dependence than the PIER signal. The results of our numerical computations are qualitatively explained in terms of the convolutions of products of third-order susceptibilities and pump field-correlation functions.
Experiments on pressure-induced extra resonances in degenerate four-wave mixing involving Zeeman coherence have been performed on Ba atoms in an argon atmosphere under conditions of large detunings from the Ba resonance line. The dependence on the detuning gives evidence for a breakdown of the impact approximation, when the laser is detuned by more than 5\ifmmode\times\else\texttimes\fi{}
1011 rad ${\mathrm{sec}}^{\ensuremath{-}1}$; the behavior can be interpreted semiquantitatively by a model based on optical collisions.
Recently one of the authors published a paper concerning the exact quantum mechanical description of pressure-induced four-wave mixing in which the exact expression of the transition probability was found.1 In this approach, a formal solution for the problem of multifield interacting with a single multilevel atom is presented by treating the fields fully quantized and the states in a dressed atomic picture. If we think of the four-wave mixing experiments as a case where the ω a , ω b , and ω c waves are sent into the medium with the fourth wave at ω p generated by the mixing, the output amplitude should be proportional to the component of the polarization fluctuating at the frequency of ω p . Based on these results, we obtained an exact quantum mechanical expression for the polarization tensor. This paper intends to explore the photon number (intensity) dependence of the polarization tensor (susceptibility) and give a comparison of the line shapes for low and high intensity of the incoming three beams. Specifically, the corresponding terms for the 31st, 32nd and 33rd terms in the Bloembergen classical expression for the susceptibility tensor will be investigated in detail.2 For no dissipation we will plot and analyze the amplitude of the polarization component at ω p .