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Physical Review A

Theory of resonances in four-wave mixing resulting from velocity-changing collisions

Michel Gorlicki, P. R. Berman, G. Khitrova

Published Jun 1, 1988• 16 citations
Publisher

Abstract

A theory of four-wave mixing including effects of velocity-changing collisions is presented. Three fields with frequencies \ensuremath{\omega}, \ensuremath{\omega}, and \ensuremath{\omega}+\ensuremath{\delta} are incident on a vapor of ``two-level'' atoms having upper state b and lower state a. Two of the fields are counterpropagating and the third (of frequency \ensuremath{\omega}+\ensuremath{\delta}) makes a small angle with one of the others. The frequency \ensuremath{\omega} is a nearly resonant (inside the Doppler width) with the a-b transition frequency. The phase-conjugate signal emitted at frequency \ensuremath{\omega}-\ensuremath{\delta} is calculated as a function of \ensuremath{\delta}. Using a simple collision model in which collisions are phase interrupting in their effect on atomic coherence and velocity-changing in their effect on level populations, we discuss the conditions under which resonances characterized by the upper or lower radiative and collision rates can be observed. Assuming that the total (a+b) state population is conserved in the absence of collisions, it is shown that velocity-changing collisions can ``open'' the system and lead to a resonance characterized by the lower-state width (convoluted with the residual Doppler width). With increasing pressure, the width of this induced resonance structure decreases monotonically. For sufficiently high pressure, the collisional redistribution of velocity classes is complete---the system ``recloses'' and the narrow resonance disappears. The interplay of the collision-induced opening, line narrowing, and reclosing of the system is discussed, as is the relationship of these narrow resonances to the so-called pressure-induced extra resonances of Bloembergen and co-workers [Indian J. Pure Appl. Phys. 16, 151 (1978); Phys. Rev. Lett. 46, 111 (1981)].

DOI
10.1103/physreva.37.4340

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Physical Review A•Nov 1, 1988•5 citations
A theory of four-wave mixing including effects of velocity-changing collisions is presented. Three fields with frequencies \ensuremath{\omega}, \ensuremath{\omega}, and \ensuremath{\omega}+\ensuremath{\delta} are incident on a vapor of two-level'' atoms having upper state b and lower state a. Two of the fields are counterpropagating and the third (of frequency \ensuremath{\omega}+\ensuremath{\delta}) makes a small angle with one of the others. The frequency \ensuremath{\omega} is a nearly resonant (inside the Doppler width) with the a-b transition frequency. The phase-conjugate signal emitted at frequency \ensuremath{\omega}-\ensuremath{\delta} is calculated as a function of \ensuremath{\delta}. Using a simple collision model in which collisions are phase interrupting in their effect on atomic coherence and velocity-changing in their effect on level populations, we discuss the conditions under which resonances characterized by the upper or lower radiative and collision rates can be observed. Assuming that the total (a+b) state population is conserved in the absence of collisions, it is shown that velocity-changing collisions can open'' the system and lead to a resonance characterized by the lower-state width (convoluted with the residual Doppler width). With increasing pressure, the width of this induced resonance structure decreases monotonically. For sufficiently high pressure, the collisional redistribution of velocity classes is complete---the system ``recloses'' and the narrow resonance disappears. The interplay of the collision-induced opening, line narrowing, and reclosing of the system is discussed, as is the relationship of these narrow resonances to the so-called pressure-induced extra resonances of Bloembergen and co-workers [Indian J. Pure Appl. Phys. 16, 151 (1978); Phys. Rev. Lett. 46, 111 (1981)].
We examine the effects of velocity-changing collisions (VCC’s) on nonlinear mixing in a Doppler-broadened vapor. We use a model in which both velocity-changing and phase-interrupting collisions are accounted for. We present explicit calculations and results for four-wave mixing in two-level systems for the case of strong collisions. We give results for both phase-conjugate and forward geometries. We discuss new features and modifications of signal line shapes due to VCC’s. The line shapes reflect the various collisional processes that occur in the system. VCC-induced line narrowing is discussed in detail.
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.
We study the effects of velocity-changing collisions (VCC's) on nearly degenerate forward four-wave mixing (FWM) in the presence of a strong pump. The calculations include the effects of both VCC's and phase-interrupting collisions. Explicit calculations and results for FWM in two-level systems for the case of strong collisions are presented in the Doppler limit. Effects of saturation on VCC-induced narrowing and those of VCC's on strong-field-induced resonances are discussed in detail.
In recent years, the collisional redistribution of radiation and collision-induced broadening of Rydberg atomic spectral lines by buffer gas perturbation have aroused the renewed interest. Rydberg atoms having a large dipole moment and long lifetime can interact with each other coherently for relatively long time, which makes them a potential candidate for quantum information processing. Besides, collisional redistribution has an important potential application in laser cooling and trapping. Based on previous experimental data, in this paper, two-nondegenerate four-wave mixing (NFWM) for studying atom collision, composed of two-photon resonant NFWM and collisional redistribution NFWM, is reported. The spectrum variation of the two-NFWM affected by the pressure, temperature, detuning and collision-broadening rate coefficient is analyzed. The principle of two-NFWM involving three incident beams is explained as follows. Consider two-NFWM in a |0-|1-|2 cascade three-level system, where states between |0 and |1 and between |1 and |2 ightangle are coupled by resonant frequencies 1 and 2 , respectively. Beam 1 with frequency 1 propagates along the direction opposite to the direction of beam 2, beams 2 and 2' have the same frequency 2, and between their directions there exists a small angle. Assuming that 1 1 and 2 2 so that 1 drives the transition from |0 to |1 while 2 drives the transition from |1 to |2, the simultaneous interactions of atoms with beams 1 and 2 will induce atomic coherence between |0 and |2 through two-photon excitation. This coherence is probed by beam 2', and as a result a two-photon resonant NFWM signal of frequency 1 is generated in the direction almost opposite to the direction of beam 2'. To avoid strong absorption at the resonant frequency of transition from |0 to |1, here the wavelength of beam1 is detuned from the exact resonance. An atom population of level |1 caused by collisional redistribution can be induced when a certain buffer gas pressure is imposed. The collisional redistribution NFWM process also exists in this case. Beam 2 drives the transition from |1 to |2 to induce an atomic coherence which is probed by beam 2' for giving rise to an atomic population grating. A collisional redistribution NFWM signal propagating along the same direction as the two-photon resonant NFWM signal is generated when beam 1 is scattered by the grating. Much information about atomic collisions can be obtained by analyzing the two NFWM signals. In a cascade three-level system composed of ground state, intermediate state and Rydberg state, and the two-NFWM can be used to investigate not only the broadening and shifting of the Rydberg level but also the collisional redistribution of the intermediate state. Unlike other experiments studying the pressure dependence of the longitudinal relaxation rate of atom states, this technique is a purely optical coherent means, and can measure the transverse relaxation rate 20 between Rydberg state and ground state as well as the pressure dependence of the transverse relaxation rate 21 between Rydberg state and intermediate state.
The effect of collisions on the resonance fluorescence spectrum of three-level atoms with a V-configuration of levels when excited by two monochromatic resonance fields has been theoretically investigated. The analysis has been carried out for the systems with a small Doppler broadening compared to the collision frequency (high buffer gas pressures) and for the general case of an arbitrary change (from complete failure to complete preservation) of the phase memory at any of the three transitions in the V-system. It has been shown that in the three-level V-type atoms excited by two monochromatic fields, the resonant fluorescence spectrum (the number of spectral lines and their widths) at one of the transitions strongly depends on the presence of resonant radiation at the adjacent transition. Under certain conditions, the line widths will be completely determined by the relaxation characteristics of the adjacent transition and, in particular, can be repeatedly narrowed with an increase in the radiation intensity at the adjacent transition. It has been shown that despite the homogeneous nature of the broadening of the absorption lines, the resonance fluorescence spectrum has a pronounced anisotropy with respect to the mutual orientation of the wave vectors of spontaneous and exciting radiation. It has been established that the line widths in the resonance fluorescence spectrum are proportional to the diffusion coefficient of the atoms interacting with radiation under certain conditions. This fact can serve as the basis for a spectroscopic method for measuring the transport frequencies of the collisions of the radiation-absorbing particles with the buffer ones. It has been shown that the effects of phase memory in the collisions lead to a strong qualitative and quantitative modification of the resonance fluorescence spectrum.
We report a series of measurements of the nearly degenerate four-wave-mixing response in atomic sodium in the presence of a helium buffer gas. The results show the line shape associated with both the ground-state and excited-state dynamics. The line shape evolves as a function of pressure from a dip at a pressure of 0 Torr to a spike at a few Torr due to the presence of collisions. The width of the spike is determined by residual Doppler broadening. At higher pressure (\ensuremath{\ge}10 Torr), the width of the spike is further narrowed below the residual Doppler width. The additional reduction is due to a form of Dicke narrowing associated with the dynamics of the lower- and upper-level excitations. The results are in qualitative agreement with a perturbation solution of the density-matrix equations which include the effects of velocity-changing collisions and state-changing collisions.