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Physical Review

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

Michael S. Feld, Ali Javan

Published Jan 10, 1969• 296 citations
Publisher

Abstract

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.

DOI
10.1103/physrev.177.540

Related papers

Laser-Induced Line-Narrowing Effects in Coupled Doppler-Broadened Transitions. II. Standing-Wave Features

B. J. Feldman, Michael S. Feld

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.

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

B. J. Feldman, Michael S. Feld

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.

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From Laser Induced Line Narrowing To Electromagnetically Induced Transparency in a Doppler-Broadened System

Ali Javan, Olga A. Kocharovskaya, Hwang Lee +1 more

Laser induced line narrowing effect in Doppler broadened systems was discovered thirty years ago. This effect can also be applied to recent experimental studies in high resolution spectroscopy or high precision measurements based on Electromagnetically Induced Transparency (EIT). In this report we derive an analytic expression for the linewidth of EIT resonance in a Doppler broadened system. It is shown here that the EIT linewidth is proportional to the Rabi frequency of the driving field and is independent of the Doppler width in a limiting case. This recovers the result found in the laser induced line narrowing effect by Feld and Javan. In the other limit, we recovers the usual power broadening case where the EIT linewidth is proportional to the intensity of the driving field and inversely proportional to the Doppler width.

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Saturation Behavior of a Doppler-Broadened Transition Involving Levels with Closely Spaced Structure

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The nonlinear absorption or gain characteristics of an optical-frequency, Doppler-broadened atomic resonance involving levels with closely spaced structure are analyzed. The level structures are assumed to be resolved with respect to their natural widths, but not necessarily with respect to the Doppler width at the optical transition. The radiation field consists of two closely spaced monochromatic frequencies lying within the Doppler width of the resonance. This type of radiation field may be obtained, for example, from a laser operating in two of its Fabry-Perot resonator modes. It is shown that, because of saturation of level populations and double-quantum Raman transitions between levels, appreciable nonlinear coupling takes place between the two fields. This coupling shows a resonance behavior when the frequency separation of the two applied fields becomes equal to the frequency splitting between two of the components which form either level structure. The width of this resonance is determined entirely by the natural widths of these two level components and not by the Doppler width of the optical transition or the natural width of other level components. When such a resonance occurs, the over-all gain or attenuation characteristics of the atomic resonance change drastically. In practice the frequency spacing of the fields may be kept constant while the level structures are tuned, e.g., magnetically. The effects are analyzed for cases of running-wave and standing-wave radiation fields. The use of this effect in precise determination of level structures as well as mode or transition coupling of a gas laser is discussed. Portions of the analysis are applicable to resonances with more general forms of inhomogeneous broadening.

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Two-photon spectroscopy. II. Effects of residual Doppler broadening

Rainer Salomaa, Stig Stenholm

For pt.I see ibid., vol.8, p.1795 (1975) where the theory of Doppler-free two-photon transitions was discussed for the case of one single laser frequency. Here, the effects of two different frequencies are considered. When the residual Doppler width of the two-photon transition is less than the natural linewidth, the previous results are essentially regained. For large residual Doppler shifts, the absorption profile is a power-broadened Lorentzian if the frequency of the probe field is larger than the frequency of the strong field. In the opposite case, the absorption peak splits because of the AC Stark effect. The high-intensity distortions are minimized when equal frequencies can be used. Power-dependent shifts do not ordinarily occur with a resonantly tuned intermediate level. Some modifications of the spectra are introduced by phase-disturbing collisions.

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Transit-time effects in power-broadened Doppler-free saturation resonances

John E. Thomas, M. J. Kelly, J.‐P. Monchalin +2 more

A density-matrix calculation of the line shape for a Doppler-broadened two-level system subjected to a plane-standing-wave laser field with a Gaussian intensity profile is presented to fifth order in perturbation theory. The primary new result is that, for fixed pressure and intensity, the power-broadening contribution to the linewidth is at a minimum when the beam radius is approximately equal to the mean free path. In addition, an analytic solution for the linewidth in the collision-dominated regime is presented for general collision parameters.

Physical Review A•Jun 1, 1977•17 citations
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.
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.
Laser induced line narrowing effect in Doppler broadened systems was discovered thirty years ago. This effect can also be applied to recent experimental studies in high resolution spectroscopy or high precision measurements based on Electromagnetically Induced Transparency (EIT). In this report we derive an analytic expression for the linewidth of EIT resonance in a Doppler broadened system. It is shown here that the EIT linewidth is proportional to the Rabi frequency of the driving field and is independent of the Doppler width in a limiting case. This recovers the result found in the laser induced line narrowing effect by Feld and Javan. In the other limit, we recovers the usual power broadening case where the EIT linewidth is proportional to the intensity of the driving field and inversely proportional to the Doppler width.
The nonlinear absorption or gain characteristics of an optical-frequency, Doppler-broadened atomic resonance involving levels with closely spaced structure are analyzed. The level structures are assumed to be resolved with respect to their natural widths, but not necessarily with respect to the Doppler width at the optical transition. The radiation field consists of two closely spaced monochromatic frequencies lying within the Doppler width of the resonance. This type of radiation field may be obtained, for example, from a laser operating in two of its Fabry-Perot resonator modes. It is shown that, because of saturation of level populations and double-quantum Raman transitions between levels, appreciable nonlinear coupling takes place between the two fields. This coupling shows a resonance behavior when the frequency separation of the two applied fields becomes equal to the frequency splitting between two of the components which form either level structure. The width of this resonance is determined entirely by the natural widths of these two level components and not by the Doppler width of the optical transition or the natural width of other level components. When such a resonance occurs, the over-all gain or attenuation characteristics of the atomic resonance change drastically. In practice the frequency spacing of the fields may be kept constant while the level structures are tuned, e.g., magnetically. The effects are analyzed for cases of running-wave and standing-wave radiation fields. The use of this effect in precise determination of level structures as well as mode or transition coupling of a gas laser is discussed. Portions of the analysis are applicable to resonances with more general forms of inhomogeneous broadening.
For pt.I see ibid., vol.8, p.1795 (1975) where the theory of Doppler-free two-photon transitions was discussed for the case of one single laser frequency. Here, the effects of two different frequencies are considered. When the residual Doppler width of the two-photon transition is less than the natural linewidth, the previous results are essentially regained. For large residual Doppler shifts, the absorption profile is a power-broadened Lorentzian if the frequency of the probe field is larger than the frequency of the strong field. In the opposite case, the absorption peak splits because of the AC Stark effect. The high-intensity distortions are minimized when equal frequencies can be used. Power-dependent shifts do not ordinarily occur with a resonantly tuned intermediate level. Some modifications of the spectra are introduced by phase-disturbing collisions.
A density-matrix calculation of the line shape for a Doppler-broadened two-level system subjected to a plane-standing-wave laser field with a Gaussian intensity profile is presented to fifth order in perturbation theory. The primary new result is that, for fixed pressure and intensity, the power-broadening contribution to the linewidth is at a minimum when the beam radius is approximately equal to the mean free path. In addition, an analytic solution for the linewidth in the collision-dominated regime is presented for general collision parameters.