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Physical Review A

Equal area property of narrow resonances induced in coupled Doppler-broadened systems by intense laser radiation

B. J. Feldman, Michael S. Feld

Published Sep 1, 1975• 15 citations
Publisher

Abstract

It is well known that the spectral line shape of the narrow change signal induced at one Doppler-broadened transition by an intense laser field resonating with a second one can be extremely complex and nonclassical in form, the exact details depending on such factors as the direction of observation relative to the propagation direction of the laser field and its spatial form (traveling wave or standing wave). Nevertheless, the area under the change signal line shape, i.e. its frequency-integrated intensity, is always the same for a given laser field, and is independent of the coupling between laser and change-signal fields. A proof of this equal area property, based on quantum-mechanical transition-rate theory, is given for a three-level system composed of degenerate or near-degenerate states. The resulting expression is also applicable to line-shape calculations for experiments which study resonance fluorescence induced by intense laser or resonance radiation or other forms of excitation.

DOI
10.1103/physreva.12.1013

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Laser-Induced Line-Narrowing Effects in Coupled Doppler-Broadened Transitions

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The line shape of a Doppler-broadened transition is dramatically altered by the presence of a laser field resonating with a second Doppler-broadened transition sharing a common level: Two narrow resonances of different widths appear superimposed upon the broad background signal at frequencies symmetrically located about the corresponding line center. The effect has already found application in a number of seemingly different though intimately related studies, including high-resolution hfs and isotope-shift determinations. The theory of the effect is developed with reference to these applications. The treatment is formulated in terms of transition rates induced by two classical fields resonantly interacting with a pair of coupled Doppler-broadened transitions of arbitrary frequencies. The perturbation approach adopted is valid for one field fully saturating its transition; the resulting line-shape expression exhibits important power-broadening effects. This approach is equivalent to the familiar density-matrix formulation, which is also presented. Various features of the resulting expression are discussed in detail as they apply to two precision spectroscopic applications, mode crossing and spontaneous emission line narrowing. The connection with previous work is also discussed.

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Effect of collisions on the resonance fluorescence spectrum

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We describe the resonance fluorescence spectrum of an atomic three-level system where two of the states are coupled by a single monochromatic laser field. The influence of the third energy level, which interacts with the two laser-coupled states only via radiative decays, is studied in detail. For a suitable choice of parameters, this system gives rise to a very narrow structure at the laser frequency in the fluorescence spectrum which is not present in the spectrum of a two-level atom. We find those parameter ranges by a numerical analysis and use the results to derive analytical expressions for the additional narrow peak. We also derive an exact expression for the peak intensity under the assumption that a random telegraph model is applicable to the system. This model and a simple spring model are then used to describe the physical origins of the additional peak. Using these results, we explain the connection between our system, a three-level system in the V configuration where both transitions are laser driven, and a related experiment that was recently reported.

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The Effect of Collisions on the Resonance Fluorescence Spectrum of Three-Level Atoms with a V-Configuration of Levels

А. И. Пархоменко, Anatolii M. Shalagin

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.

Optics and Spectroscopy•Dec 1, 2021•1 citation
It is well known that the spectral line shape of the narrow change signal induced at one Doppler-broadened transition by an intense laser field resonating with a second one can be extremely complex and nonclassical in form, the exact details depending on such factors as the direction of observation relative to the propagation direction of the laser field and its spatial form (traveling wave or standing wave). Nevertheless, the area under the change signal line shape, i.e. its frequency-integrated intensity, is always the same for a given laser field, and is independent of the coupling between laser and change-signal fields. A proof of this equal area property, based on quantum-mechanical transition-rate theory, is given for a three-level system composed of degenerate or near-degenerate states. The resulting expression is also applicable to line-shape calculations for experiments which study resonance fluorescence induced by intense laser or resonance radiation or other forms of excitation.
The line shape of a Doppler-broadened transition is dramatically altered by the presence of a laser field resonating with a second Doppler-broadened transition sharing a common level: Two narrow resonances of different widths appear superimposed upon the broad background signal at frequencies symmetrically located about the corresponding line center. The effect has already found application in a number of seemingly different though intimately related studies, including high-resolution hfs and isotope-shift determinations. The theory of the effect is developed with reference to these applications. The treatment is formulated in terms of transition rates induced by two classical fields resonantly interacting with a pair of coupled Doppler-broadened transitions of arbitrary frequencies. The perturbation approach adopted is valid for one field fully saturating its transition; the resulting line-shape expression exhibits important power-broadening effects. This approach is equivalent to the familiar density-matrix formulation, which is also presented. Various features of the resulting expression are discussed in detail as they apply to two precision spectroscopic applications, mode crossing and spontaneous emission line narrowing. The connection with previous work is also discussed.
Previous theoretical results on the influence of a laser on the line shape of a coupled transition-laser-induced line narrowing-have been restricted to the case where the laser is detuned from the center of its atomic gain profile or is in the form of a traveling wave. This paper extends those results to include the case where the laser is an intense standing-wave field tunable to the center of its atomic gain profile (conditions for Lamb dip). The effect may be observed either in transmission, by probing the coupled transition with a weak traveling-wave field coaxial with the laser field, or else in spontaneous emission from the coupled transition viewed along the axis of the laser field. It is now well known that for a laser detuned from the center of its atomic gain profile, two narrow Lorentzian resonances of different widths appear superimposed upon the broad background signal at frequencies symmetrically located about the corresponding line center. When the laser is tuned to the center of its gain profile, however, additional fine structure develops. This structure, which is particularly significant when the laser field is intense, may have important applications in highresolution spectroscopy and laser-frequency stabilization. In this paper the laser frequency may be smaller or larger than the frequency of the coupled transition. In the latter case an intense laser introduces additional splitting effects, even when the laser is detuned. Splitting effects due to weakly saturating laser fields are also discussed. The problem is formulated by expanding elements of the ensemble-averaged density matrix in an infinite series of spatial Fourier components. A perturbation technique is employed, valid for a weak probe field and a standing-wave field of arbitrary intensity. One obtains an expression for emission induced by the probe field due to atoms moving with one velocity, written in terms of continued fractions in the general case and with Bessel functions in an important special case. This expression is integrated over the atomic velocity distribution by means of a computer to obtain the total emission due to atoms moving with all velocities. In some cases the integrated expressions may be written in closed algebraic form. A detailed discussions of line shapes and of the physical processes involved is included.
The effect of collisions on the resonance fluorescence spectrum of two-level atoms excited by monochromatic resonance radiation is studied. Analysis is performed for systems where the Doppler broadening is small compared to the collision frequency (high buffer gas pressures) and for the general case where collisions arbitrarily change the phase of the radiation-induced dipole moment (from completely interrupted to completely unaffected phase of the dipole moment). Both at a relatively low and at a high excitation radiation intensity, the resonance fluorescence spectrum is shown to depend on whether the two-level system is closed or open. This is especially true for the narrow unshifted Rayleigh scattering line. It is shown that, although the absorption line is homogeneously broadened, the resonance fluorescence spectrum exhibits a clearly pronounced anisotropy. In a direction close to the direction of propagation of the excitation radiation, the Rayleigh scattering line is maximally narrowed. Under certain conditions (that can easily be created in experiments), the width of this line is proportional to the diffusion coefficient of atoms interacting with the radiation.
We present a theoretical and experimental study of the line shape of resonant four-wave mixing induced by broad-bandwidth laser radiation that revises the theory of Meacher, Smith, Ewart, and Cooper (MSEC) [Phys. Rev. A 46, 2718 (1992)]. We adopt the same method as MSEC but correct for an invalid integral used to average over the distribution of atomic velocities. The revised theory predicts a Voigt line shape composed of a homogeneous, Lorentzian component, defined by the collisional rate \ensuremath{\Gamma}, and an inhomogeneous, Doppler component, which is a squared Gaussian. The width of the inhomogeneous component is reduced by a factor of \ensuremath{\surd}2 compared to the simple Doppler width predicted by MSEC. In the limit of dominant Doppler broadening, the width of the homogeneous component is predicted to be 4\ensuremath{\Gamma}, whereas in the limit of dominant homogeneous broadening, the predicted width is 2\ensuremath{\Gamma}. An experimental measurement is reported of the line shape of the four-wave-mixing signal using a broad-bandwidth, ``modeless,'' laser resonant with the Q1{\mathit{Q}}_{1}Q1​(6) line of the A2{\mathrm{}}^{2}2\ensuremath{\Sigma}-X2{\mathrm{}}^{2}2\ensuremath{\Pi}(0,0) system of the hydroxyl radical. The measured widths of the Voigt components were found to be consistent with the predictions of the revised theory. \textcopyright{} 1996 The American Physical Society.
We describe the resonance fluorescence spectrum of an atomic three-level system where two of the states are coupled by a single monochromatic laser field. The influence of the third energy level, which interacts with the two laser-coupled states only via radiative decays, is studied in detail. For a suitable choice of parameters, this system gives rise to a very narrow structure at the laser frequency in the fluorescence spectrum which is not present in the spectrum of a two-level atom. We find those parameter ranges by a numerical analysis and use the results to derive analytical expressions for the additional narrow peak. We also derive an exact expression for the peak intensity under the assumption that a random telegraph model is applicable to the system. This model and a simple spring model are then used to describe the physical origins of the additional peak. Using these results, we explain the connection between our system, a three-level system in the V configuration where both transitions are laser driven, and a related experiment that was recently reported.
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.