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Physical Review A

Nonlinear effects in optical pumping of atoms by a high-intensity multimode gas laser. II. Exact theory for small angular momenta

M. Ducloy

Published Mar 1, 1974• 27 citations
Publisher

Abstract

In a previous paper, I have presented a general theory of the optical pumping of atoms by a polarized multimode-laser beam, in the presence of a magnetic field. Equations of motion, valid at arbitrary laser intensities for the density matrix of the atomic system, have been obtained. In this paper, these equations are exactly solved for a linearly $\ensuremath{\sigma}$-polarized laser and levels having small angular momenta. More precisely, I consider the laser transitions ${J}_{b}=1\ensuremath{\rightarrow}{J}_{a}=0$, ${J}_{b}=1\ensuremath{\rightarrow}{J}_{a}=1$, and ${J}_{b}=1\ensuremath{\rightarrow}{J}_{a}=2$. Two particular results are emphasized: (i) For $J=1\ensuremath{-}J=0$ and $J=1\ensuremath{-}J=1$ transitions and for the $J=2$ level of a $J=1\ensuremath{-}J=2$ transition, the laser-induced Hanle effects keep a Lorentzian shape, independent of the laser intensity. For the $J=1\ensuremath{-}J=1$ transition, it is shown that the depolarizing relaxation processes play a leading part in the coupling induced by the laser between the transverse alignments of the two levels. On the other hand, the power broadenings of the Hanle effects are shown to be similar. For the $J=1$ level of a $J=1\ensuremath{-}J=2$ transition, the Hanle-effect shape presents a departure from the Lorentzian one, owing to a coupling with the laser-induced hexadecapole moment in the $J=2$ level. (ii) The populations of the levels exhibit a "zero-field saturation resonance" which is due to the coupling with the Zeeman coherences. These resonances, which reproduce the Hanle effects of the transition, can be observed on the $\ensuremath{\pi}$-polarized fluorescence from the levels. In general, these resonances appear as a saturation effect, i.e., they reduce the laser-induced fluorescence of the levels in zero magnetic field. However, for the ${J}_{b}=1\ensuremath{\rightarrow}{J}_{a}=2$ transition, the ${J}_{a}=2\ensuremath{\rightarrow}{J}_{f}=2 \ensuremath{\pi}$ fluorescence presents an anomalous behavior; the saturation resonance increases the zero-field laser-induced fluorescence. The theoretical study shows the prominent part played by the value of the ${J}_{b}=1$ level lifetime in the interpretation of this anomaly. Other results, such as the laser-induced depolarization of the fluorescence, are also obtained. All the theoretical predictions have been experimentally checked and will be presented in forthcoming papers.

DOI
10.1103/physreva.9.1319

Related papers

Nonlinear Effects in Optical Pumping of Atoms by a High-Intensity Multimode Gas Laser. General Theory

M. Ducloy

The optical pumping of atoms by a multimode gas laser, in the presence of a magnetic field, is studied theoretically. The atoms are described by their density matrix, which is expanded on an irreducible tensorial set. The atomic relaxation is assumed to be isotropic. In order to avoid the usual perturbation theory, we use the so-called "Broad-Line approximation" (BLA). BLA is valid when the width of the "Bennett hole" created by one laser mode in the velocity distribution of the excited atoms is comparable to the spacing between modes; under these conditions, the atomic response does not depend on the velocity and the multimode laser irradiation is equivalent to a broad-line excitation. For the atomic system, BLA leads to a set of coupled equations which is valid at arbitrary intensities of the laser field and which depends on this field through a unique parameter, $\ensuremath{\gamma}$. This parameter can be understood as a laser-induced transition probability. In this article, we analyze the nonlinear effects which can be deduced from this theory, for any value of the angular momenta involved in the laser transition: Hanle-effect broadening, alignment coupling, saturation resonances on the populations are shown. The exact calculations, valid at arbitrary laser intensities for $J=1\ensuremath{\leftrightarrow}J=0$, $J=1\ensuremath{\leftrightarrow}J=1$, and $J=1\ensuremath{\leftrightarrow}J=2$ transitions, and the corresponding experimental results will be presented in forthcoming papers.

Physical Review A•Oct 1, 1973•83 citations

Non-linear effects in optical pumping with lasers. I. General theory of the classical limit for levels of large angular momenta

M. Ducloy

The optical pumping of high J levels with a broad-band CW laser is studied theoretically. Exact non-perturbative solutions are obtained by means of a Fourier development of the response of the irradiated medium. This leads to such theoretical predictions as the depolarization of the fluorescence for high laser intensities, the power broadening of the Hanle effect and the appearance of a zero-field saturation resonance in the pi fluorescence. All these theoretical predictions are finally compared with recent experiments on the optical pumping of molecules especially Na 2 and I 2 .

Journal of Physics B Atomic and Molecular Physics•Feb 21, 1976•25 citations

Nonlinear effects in optical pumping with lasers. II. Possible radiative narrowing of the Hanle resonance at the classical limit

M. Ducloy

For pt.I see ibid., vol.9, p.357 (1976). A theory of the optical pumping of high-J molecule levels with a broad-band CW laser has previously been developed. The linewidth of the Hanle effect is analysed in the present paper for two particular cases in which an exact integration is possible. These cases are: (i) gT (where g is the Lande factor and T the lifetime) is the same for the two levels; and (ii) one of the Lande factors vanishes. In general, the Hanle resonance is power-broadened for high laser intensities. However, in the case of a zero Lande factor of the ground state, the theory predicts a radiative narrowing of the Hanle effect. It is shown that this most unusual feature is connected to the fact that, in the latter case, the physical observables of the resonance level may get the ground-state lifetime, when the transition is saturated.

Journal of Physics B Atomic and Molecular Physics•Apr 1, 1976•0 citations

Saturation resonances by magnetic mode crossing in optical pumping with a multimode gas laser

Michel L. Dumont

The fluorescence light emitted by atoms (Ne) optically pumped with a multimode laser beam exhibits a resonance each time the Zeeman splitting is equal to the frequency difference between two modes. The experimental study shows that these resonances are very sensitive to the relative phase of modes and that their width is approximately equal to the Hanle effect width. A theoretical interpretation is given with the help of a perturbation calculation. Two phenomena produce resonances : 1) A Population Effect (PE) which is resonant when the σ + component of one mode and the σ- component of another interact with atoms of same velocity (hole crossing). The width of these resonances is 2 Γ'ab (natural width broadened by collisions). 2) A Zeeman Coherence Effect (ZCE) : the action of a pair of modes (ν, σ +) and (μ, σ-) produces (at 2nd order) transverse alignment modulated at the beat frequency ων — ω μ and resonant when the Zeeman splitting is equal to that frequency ; by interaction with a second pair of modes (λ, σ-) and (κ, σ+) (ων —ω μ + ωλ — ωκ = 0), this alignment produces unmodulated longitudinal quantities (4th order) which exhibit, as the magnetic field is scanned, a resonance whose width is close to that of the Hanle curve (Γ b(2)). In our experimental conditions (close modes : Γ'ab≳ Δω > Γ b(2)), the resonances of the first kind are not resolved and the observed resonances are only of the second type's which arevery sensitive to the phases of modes. We also discuss the possibility of using these resonances to measure Landé g factors.

Journal de physique•Jan 1, 1972•31 citations

Magnetic field and pressure effects in a saturated gas laser amplifier

Robert T. Menzies

Theoretical and experimental studies of a gas laser amplifier are presented, assuming the amplifier is operating with a saturating optical frequency signal. The analysis is primarily concerned with the effects of the gas pressure and the presence of an axial magnetic field on the characteristics of the amplifying medium. Semiclassical radiation theory is used, along with a density matrix description of the atomic medium which relates the motion of single atoms to the macroscopic observables. A two-level description of the atom, using phenomenological source rates and decay rates, forms the basis of our analysis of the gas laser medium. Pressure effects are taken into account to a large extent through suitable choices of decay rate parameters. Two methods for calculating the induced polarization of the atomic medium are used. The first method utilizes a perturbation expansion which is valid for signal intensities which barely reach saturation strength, and it is quite general in applicability. The second method is valid for arbitrarily strong signals, but it yields tractable solutions only for zero magnetic field or for axial magnetic fields large enough such that the Zeeman splitting is much larger than the power broadened homogeneous linewidth of the laser transition. The effects of pressure broadening of the homogeneous spectral linewidth are included in both the weak-signal and strong-signal theories; however the effects of Zeeman sublevel-mixing collisions are taken into account only in the weak-signal theory. The behavior of a He-Ne gas laser amplifier in the presence of an axial magnetic field has been studied experimentally by measuring gain and Faraday rotation of linearly polarized resonant laser signals for various values of input signal intensity, and by measuring nonlinearity - induced anisotropy for elliptically polarized resonant laser signals of various input intensities. Two high-gain transitions in the 3.39-μ region were used for study: a J = 1 to J = 2 (3s2 → 3p4) transition and a J = 1 to J = 1 (3s2 → 3p2) transition. The input signals were tuned to the centers of their respective resonant gain lines. The experimental results agree quite well with corresponding theoretical expressions which have been developed to include the nonlinear effects of saturation strength signals. The experimental results clearly show saturation of Faraday rotation, and for the J = 1 t o J = 1 transition a Faraday rotation reversal and a traveling wave gain dip are seen for small values of axial magnetic field. The nonlinearity induced anisotropy shows a marked dependence on the gas pressure in the amplifier tube for the J = 1 to J = 2 transition; this dependence agrees with the predictions of the general perturbational or weak signal theory when allowances are made for the effects of Zeeman sublevel-mixing collisions. The results provide a method for measuring the upper (neon 3s2) level quadrupole moment decay rate, the dipole moment decay rates for the 3s2 → 3p4 and 3s2 → 3p2 transitions, and the effects of various types of collision processes on these decay rates.

•Aug 12, 2015•1 citation

Optical Hanle effect

V.Paul Kaftandjian, Christian Delsart, J. Keller

The optical Hanle effect (light-shift-induced zero-field level crossing) has been investigated theoretically and experimentally. In the case of a $J=0\ensuremath{\rightarrow}1\ensuremath{\rightarrow}0$ three-level system and of a $J=0\ensuremath{\rightarrow}1$ two-level system, the resonance line shape has been obtained using a nonlinear-response-function method. Approximate expressions, valid under the conditions for the observation of light shifts, are obtained and compared with exact calculations as well as with the corresponding expression for the magnetic Hanle effect. As concerns the weak laser beam which produces the coherent excitation of atomic substates, we have calculated the linear response in the limiting case of monochromatic and of broad-band excitation. The experimental investigation has been performed for the Ba resonance line using two cw dye lasers at $\ensuremath{\lambda}=5535$ \AA{} and an atomic beam. The absorption- and dispersion-shaped level crossing resonances have been observed, for narrow- and broad-band excitation, by varying the power of the strong nonresonant laser beam. We have checked that the line shapes are only dependent upon the reduced variable $\frac{{P}_{L}}{\ensuremath{\delta}}$ (${P}_{L}$; beam power; $\ensuremath{\delta}$: frequency detuning). Using the theoretical expressions, we have tried to fit the experimental curves. Provided that the Gaussian distribution of the beams is taken into account, we have obtained a good agreement between theory and experiment for the whole set of experimental data.

Physical Review A•Mar 1, 1981•13 citations
In a previous paper, I have presented a general theory of the optical pumping of atoms by a polarized multimode-laser beam, in the presence of a magnetic field. Equations of motion, valid at arbitrary laser intensities for the density matrix of the atomic system, have been obtained. In this paper, these equations are exactly solved for a linearly \ensuremathσ\ensuremath{\sigma}\ensuremathσ-polarized laser and levels having small angular momenta. More precisely, I consider the laser transitions Jb=1\ensuremath→Ja=0{J}_{b}=1\ensuremath{\rightarrow}{J}_{a}=0Jb​=1\ensuremath→Ja​=0, Jb=1\ensuremath→Ja=1{J}_{b}=1\ensuremath{\rightarrow}{J}_{a}=1Jb​=1\ensuremath→Ja​=1, and Jb=1\ensuremath→Ja=2{J}_{b}=1\ensuremath{\rightarrow}{J}_{a}=2Jb​=1\ensuremath→Ja​=2. Two particular results are emphasized: (i) For J=1\ensuremath−J=0J=1\ensuremath{-}J=0J=1\ensuremath−J=0 and J=1\ensuremath−J=1J=1\ensuremath{-}J=1J=1\ensuremath−J=1 transitions and for the J=2J=2J=2 level of a J=1\ensuremath−J=2J=1\ensuremath{-}J=2J=1\ensuremath−J=2 transition, the laser-induced Hanle effects keep a Lorentzian shape, independent of the laser intensity. For the J=1\ensuremath−J=1J=1\ensuremath{-}J=1J=1\ensuremath−J=1 transition, it is shown that the depolarizing relaxation processes play a leading part in the coupling induced by the laser between the transverse alignments of the two levels. On the other hand, the power broadenings of the Hanle effects are shown to be similar. For the J=1J=1J=1 level of a J=1\ensuremath−J=2J=1\ensuremath{-}J=2J=1\ensuremath−J=2 transition, the Hanle-effect shape presents a departure from the Lorentzian one, owing to a coupling with the laser-induced hexadecapole moment in the J=2J=2J=2 level. (ii) The populations of the levels exhibit a "zero-field saturation resonance" which is due to the coupling with the Zeeman coherences. These resonances, which reproduce the Hanle effects of the transition, can be observed on the \ensuremathπ\ensuremath{\pi}\ensuremathπ-polarized fluorescence from the levels. In general, these resonances appear as a saturation effect, i.e., they reduce the laser-induced fluorescence of the levels in zero magnetic field. However, for the Jb=1\ensuremath→Ja=2{J}_{b}=1\ensuremath{\rightarrow}{J}_{a}=2Jb​=1\ensuremath→Ja​=2 transition, the Ja=2\ensuremath→Jf=2\ensuremathπ{J}_{a}=2\ensuremath{\rightarrow}{J}_{f}=2 \ensuremath{\pi}Ja​=2\ensuremath→Jf​=2\ensuremathπ fluorescence presents an anomalous behavior; the saturation resonance increases the zero-field laser-induced fluorescence. The theoretical study shows the prominent part played by the value of the Jb=1{J}_{b}=1Jb​=1 level lifetime in the interpretation of this anomaly. Other results, such as the laser-induced depolarization of the fluorescence, are also obtained. All the theoretical predictions have been experimentally checked and will be presented in forthcoming papers.
The optical pumping of atoms by a multimode gas laser, in the presence of a magnetic field, is studied theoretically. The atoms are described by their density matrix, which is expanded on an irreducible tensorial set. The atomic relaxation is assumed to be isotropic. In order to avoid the usual perturbation theory, we use the so-called "Broad-Line approximation" (BLA). BLA is valid when the width of the "Bennett hole" created by one laser mode in the velocity distribution of the excited atoms is comparable to the spacing between modes; under these conditions, the atomic response does not depend on the velocity and the multimode laser irradiation is equivalent to a broad-line excitation. For the atomic system, BLA leads to a set of coupled equations which is valid at arbitrary intensities of the laser field and which depends on this field through a unique parameter, $\ensuremath{\gamma}$. This parameter can be understood as a laser-induced transition probability. In this article, we analyze the nonlinear effects which can be deduced from this theory, for any value of the angular momenta involved in the laser transition: Hanle-effect broadening, alignment coupling, saturation resonances on the populations are shown. The exact calculations, valid at arbitrary laser intensities for $J=1\ensuremath{\leftrightarrow}J=0$, $J=1\ensuremath{\leftrightarrow}J=1$, and $J=1\ensuremath{\leftrightarrow}J=2$ transitions, and the corresponding experimental results will be presented in forthcoming papers.
The optical pumping of high J levels with a broad-band CW laser is studied theoretically. Exact non-perturbative solutions are obtained by means of a Fourier development of the response of the irradiated medium. This leads to such theoretical predictions as the depolarization of the fluorescence for high laser intensities, the power broadening of the Hanle effect and the appearance of a zero-field saturation resonance in the pi fluorescence. All these theoretical predictions are finally compared with recent experiments on the optical pumping of molecules especially Na 2 and I 2 .
For pt.I see ibid., vol.9, p.357 (1976). A theory of the optical pumping of high-J molecule levels with a broad-band CW laser has previously been developed. The linewidth of the Hanle effect is analysed in the present paper for two particular cases in which an exact integration is possible. These cases are: (i) gT (where g is the Lande factor and T the lifetime) is the same for the two levels; and (ii) one of the Lande factors vanishes. In general, the Hanle resonance is power-broadened for high laser intensities. However, in the case of a zero Lande factor of the ground state, the theory predicts a radiative narrowing of the Hanle effect. It is shown that this most unusual feature is connected to the fact that, in the latter case, the physical observables of the resonance level may get the ground-state lifetime, when the transition is saturated.
The fluorescence light emitted by atoms (Ne) optically pumped with a multimode laser beam exhibits a resonance each time the Zeeman splitting is equal to the frequency difference between two modes. The experimental study shows that these resonances are very sensitive to the relative phase of modes and that their width is approximately equal to the Hanle effect width. A theoretical interpretation is given with the help of a perturbation calculation. Two phenomena produce resonances : 1) A Population Effect (PE) which is resonant when the σ + component of one mode and the σ- component of another interact with atoms of same velocity (hole crossing). The width of these resonances is 2 Γ'ab (natural width broadened by collisions). 2) A Zeeman Coherence Effect (ZCE) : the action of a pair of modes (ν, σ +) and (μ, σ-) produces (at 2nd order) transverse alignment modulated at the beat frequency ων — ω μ and resonant when the Zeeman splitting is equal to that frequency ; by interaction with a second pair of modes (λ, σ-) and (κ, σ+) (ων —ω μ + ωλ — ωκ = 0), this alignment produces unmodulated longitudinal quantities (4th order) which exhibit, as the magnetic field is scanned, a resonance whose width is close to that of the Hanle curve (Γ b(2)). In our experimental conditions (close modes : Γ'ab≳ Δω > Γ b(2)), the resonances of the first kind are not resolved and the observed resonances are only of the second type's which arevery sensitive to the phases of modes. We also discuss the possibility of using these resonances to measure Landé g factors.
Theoretical and experimental studies of a gas laser amplifier are presented, assuming the amplifier is operating with a saturating optical frequency signal. The analysis is primarily concerned with the effects of the gas pressure and the presence of an axial magnetic field on the characteristics of the amplifying medium. Semiclassical radiation theory is used, along with a density matrix description of the atomic medium which relates the motion of single atoms to the macroscopic observables. A two-level description of the atom, using phenomenological source rates and decay rates, forms the basis of our analysis of the gas laser medium. Pressure effects are taken into account to a large extent through suitable choices of decay rate parameters. Two methods for calculating the induced polarization of the atomic medium are used. The first method utilizes a perturbation expansion which is valid for signal intensities which barely reach saturation strength, and it is quite general in applicability. The second method is valid for arbitrarily strong signals, but it yields tractable solutions only for zero magnetic field or for axial magnetic fields large enough such that the Zeeman splitting is much larger than the power broadened homogeneous linewidth of the laser transition. The effects of pressure broadening of the homogeneous spectral linewidth are included in both the weak-signal and strong-signal theories; however the effects of Zeeman sublevel-mixing collisions are taken into account only in the weak-signal theory. The behavior of a He-Ne gas laser amplifier in the presence of an axial magnetic field has been studied experimentally by measuring gain and Faraday rotation of linearly polarized resonant laser signals for various values of input signal intensity, and by measuring nonlinearity - induced anisotropy for elliptically polarized resonant laser signals of various input intensities. Two high-gain transitions in the 3.39-μ region were used for study: a J = 1 to J = 2 (3s2 → 3p4) transition and a J = 1 to J = 1 (3s2 → 3p2) transition. The input signals were tuned to the centers of their respective resonant gain lines. The experimental results agree quite well with corresponding theoretical expressions which have been developed to include the nonlinear effects of saturation strength signals. The experimental results clearly show saturation of Faraday rotation, and for the J = 1 t o J = 1 transition a Faraday rotation reversal and a traveling wave gain dip are seen for small values of axial magnetic field. The nonlinearity induced anisotropy shows a marked dependence on the gas pressure in the amplifier tube for the J = 1 to J = 2 transition; this dependence agrees with the predictions of the general perturbational or weak signal theory when allowances are made for the effects of Zeeman sublevel-mixing collisions. The results provide a method for measuring the upper (neon 3s2) level quadrupole moment decay rate, the dipole moment decay rates for the 3s2 → 3p4 and 3s2 → 3p2 transitions, and the effects of various types of collision processes on these decay rates.
The optical Hanle effect (light-shift-induced zero-field level crossing) has been investigated theoretically and experimentally. In the case of a $J=0\ensuremath{\rightarrow}1\ensuremath{\rightarrow}0$ three-level system and of a $J=0\ensuremath{\rightarrow}1$ two-level system, the resonance line shape has been obtained using a nonlinear-response-function method. Approximate expressions, valid under the conditions for the observation of light shifts, are obtained and compared with exact calculations as well as with the corresponding expression for the magnetic Hanle effect. As concerns the weak laser beam which produces the coherent excitation of atomic substates, we have calculated the linear response in the limiting case of monochromatic and of broad-band excitation. The experimental investigation has been performed for the Ba resonance line using two cw dye lasers at $\ensuremath{\lambda}=5535$ \AA{} and an atomic beam. The absorption- and dispersion-shaped level crossing resonances have been observed, for narrow- and broad-band excitation, by varying the power of the strong nonresonant laser beam. We have checked that the line shapes are only dependent upon the reduced variable $\frac{{P}_{L}}{\ensuremath{\delta}}$ (PL{P}_{L}PL​; beam power; $\ensuremath{\delta}$: frequency detuning). Using the theoretical expressions, we have tried to fit the experimental curves. Provided that the Gaussian distribution of the beams is taken into account, we have obtained a good agreement between theory and experiment for the whole set of experimental data.