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Journal of the Optical Society of America B

Propagation of modulated optical fields through saturable-absorbing media: a general theory of modulation spectroscopy

Mark A. Kramer, Robert W. Boyd, Lloyd W. Hillman, Carlos R. Stroud

Published Sep 1, 1985• 22 citations
Publisher

Abstract

The propagation of a weakly modulated light beam through a nonlinear material is treated. The optical field representing such a beam consists of a strong carrier-frequency component and two weak, symmetrically displaced sidebands that combine to form a field, which may be purely amplitude modulated (AM), frequency modulated (FM), or some combination of these two modulation forms. It is shown that, for any optical nonlinearity, two modulation forms exist that have the property that the form of modulation is invariant under propagation of the beam. If a modulation form other than one of these natural modes is injected into the nonlinear medium, the modulation form will change as the beam propagates, asymptotically approaching the natural mode that experiences the lower attenuation. Explicit expressions for these natural modes are presented for the case in which the nonlinear medium can be modeled as a collection of two-level atoms. For the special case of an on-resonance pump beam, the natural modes correspond to pure amplitude modulation and pure frequency modulation. This formalism provides a general description of saturation spectroscopy for both AM and FM fields. Formulas are derived for the rate at which a pure FM beam is converted to an AM beam owing to its interaction with a two-level atomic medium. We also consider the variation that is due to propagation of the depth of modulation of an AM wave interacting resonantly with two-level atoms. The formalism predicts the existence of spectral features whose shape depends sensitively on the internal relaxation processes of the material. Experimental spectra are presented for ruby, alexandrite, and fluorescein in glass and are interpreted.

DOI
10.1364/josab.2.001444

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Annual Meeting Optical Society of America•Jan 1, 1990•0 citations
The propagation of a weakly modulated light beam through a nonlinear material is treated. The optical field representing such a beam consists of a strong carrier-frequency component and two weak, symmetrically displaced sidebands that combine to form a field, which may be purely amplitude modulated (AM), frequency modulated (FM), or some combination of these two modulation forms. It is shown that, for any optical nonlinearity, two modulation forms exist that have the property that the form of modulation is invariant under propagation of the beam. If a modulation form other than one of these natural modes is injected into the nonlinear medium, the modulation form will change as the beam propagates, asymptotically approaching the natural mode that experiences the lower attenuation. Explicit expressions for these natural modes are presented for the case in which the nonlinear medium can be modeled as a collection of two-level atoms. For the special case of an on-resonance pump beam, the natural modes correspond to pure amplitude modulation and pure frequency modulation. This formalism provides a general description of saturation spectroscopy for both AM and FM fields. Formulas are derived for the rate at which a pure FM beam is converted to an AM beam owing to its interaction with a two-level atomic medium. We also consider the variation that is due to propagation of the depth of modulation of an AM wave interacting resonantly with two-level atoms. The formalism predicts the existence of spectral features whose shape depends sensitively on the internal relaxation processes of the material. Experimental spectra are presented for ruby, alexandrite, and fluorescein in glass and are interpreted.
A theoretical study of amplitude (AM) and frequency (FM) modulation components of an optical wave interacting resonantly with a homogeneously broadened two-level system is presented. It is shown that the AM component is usually less attenuated than the FM component; however, under conditions which depend on the modulation frequency, relaxation times, and the saturation parameter, the reverse may occur. In strongly saturated media the AM component can be amplified, a process limited by the depletion of the carrier intensity as the wave propagates in the absorber. The two- and three-wave cases of unidirectional saturation spectroscopy are considered and the effects of depletion are discussed. In the two-wave (single-probe) case a third wave is generated which substantially modifies the absorption profile for the probe. An analysis is included of the sideband evolution in a laser with an intracavity saturable absorber. By analyzing the problem in the frequency domain, some new insights concerning the role of the saturable absorber in passively mode-locked lasers are presented.
The purpose of this work was to investigate coherence effects in the interaction of two counterpropagating electromagnetic waves with the atoms of a gas, in the case in which one of the waves is weak and frequency modulated, while the other is sufficiently intense to cause saturation. Solving the equations for the density matrix in first-order perturbation theory, the authors obtained in analytic form the real part of the susceptibility integrated over the atom's velocity, expressed in terms of the rate equation model (REM) predictions plus the coherence corrections. The relaxation constants of the levels involved in the transition were kept different in order to allow a wider range of applications of the results. Calculated line shapes related either to the frequency-modulated (FM) sideband or to the ordinary dispersion techniques are presented. The REM approximation and the coherence corrections are shown in detail for an optical line which is of interest for frequency standard investigations.
We have investigated the interaction between bichromatic optical fields and atomic transitions. We have considered both the interaction of a saturating bichromatic field in the form of a 100% amplitude-modulated field resonantly interacting with a single atomic transition as well as the interaction of a pair of 100% amplitude-modulated fields with two coupled atomic transitions. In our studies of a single atomic transition resonantly excited by a 100% amplitude-modulated field we have used a fully quantum-electrodynamical analysis to model the Autler-Townes effect induced by a bichromatic optical field. We find that the effect induced by a bichromatic field is markedly different from the effect produced by a monochromatic exciting field. We have derived analytic expressions for the bichromatic Autler-Townes absorption spectrum. The absorption spectrum consists of equally spaced lines spaced by the modulation frequency. The linewidths of neighboring lines alternate as functions of the field strength. Experimentally, we observed this spectrum for both resonant and detuned 100% amplitude-modulated driving fields by monitoring the absorption of a weak monochromatic field as it was tuned about the resonance frequency of the 3²P₃/₂(F = 3, mF = 3) ↔ 4²D₅/₂(F = 4, mF = 4) transition while driving the 3²S₁/₂(F = 2, mF = 2) ↔ 3²P₃/₂(F = 3, mF = 3) transition with a saturating 100% amplitude-modulated field. We found excellent agreement between our predicted and measured spectra. We then investigated the resonant interaction between a pair of 100% amplitude-modulated fields and two atomic transitions sharing a common atomic level. We considered both a three-level atomic cascade system and a three-level atomic lambda system. We examined the effect that the relative phase between the two modulations has on the rate at which the modulated fields are absorbed. We find that the saturated time-averaged field absorption exhibits parametric resonances in both the cascade and lambda systems. The time-averaged absorption is strongly dependent upon the relative phase of modulation between the two fields and for certain phase differences the time-averaged absorption can be enhanced over the maximum saturated absorption experienced by cw fields of the same time-averaged intensities. We also find that the stationary atomic response exhibits periodic oscillations and for the cascade system periodic two-photon inversions of up to 40% can be achieved. We further find dark absorption resonances as a function of phase in the lambda system. We analyze the results from the point of view of semi-classical adiabatic dressed states.
A novel phase-modulation technique which permits subkilohertz-laser stability and new levels of precision in laser spectroscopy was reported recently. For spectroscopy, the basic arrangement consists of a combination of an optical pump and a probe field which is phase modulated. The pump prepares the atomic sample by burning a narrow hole within the atom's inhomogeneous line shape, and the probe beam samples the prepared hole when its modulation sidebands are swept into resonance. Off resonance, the probe is balanced as pairs of sidebands produce heterodyne beat signals of opposite phase which just cancel. On resonance, the balance is upset and yields a nonvanishing beat signal with a Lorentzian absorption or dispersion line shape and with residual noise approaching the shot noise limit. Here we investigate the theory of phase-modulation spectroscopy. We treat the nonlinear response of an atomic two-level quantum system subject to an intense pump and a weak copropagating or counterpropagating phase-modulated probe beam. The density-matrix equations of motion are solved by a Laplace-transform method and by the novel use of a translation operator which allows the infinite hierarchy of coupled equations to close. A solution equivalent to the rate-equation result is developed and coherence corrections are found which predict new resonances that have just been detected in this laboratory. The delayed pump-probe technique encountered in solid-state laser spectroscopy is analyzed in this context for two- and three-level quantum systems. The response of a Fabry-Perot cavity to a phase-modulated light wave is examined also and reveals an unexpected absorption feature.
On-resonance self-action of a beam with periodically modulated amplitude in a two-level saturable absorber is studied numerically. When the period of modulation is comparable with relaxation times, one cannot describe the medium by means of susceptibility, and the response of the medium to the amplitude variation is not immediate. We solve the Bloch equations in each point of the medium to find this response correctly. Transient behavior followed by stable oscillations of population difference and polarization vector is shown to depend strongly on the frequency and amplitude of modulation. Beam propagation is considered using a simplified model of a thin absorber followed by free space, the propagation distance being small compared with the modulation wavelength. Manifestations of non-stationary response of the medium in the output intensity behavior are analyzed.
The interaction of a strong bichromatic field with a two-level atom has been the subject of numerous experimental and theoretical investigations. We performed an experimental study of the Interaction of an intense 100% amplitude-modulated (AM) field with an ensemble of homogeneously broadened two-level atoms. An optically pumped sodium atomic beam is used as the atomic medium. The field is created by interfering two intense frequency-stabilized laser fields. The frequency of one field is held fixed while another field of equal amplitude is scanned in frequency. The beat frequency produced by interfering the two laser fields is equal to twice the modulation frequency of a 100% AM field. We monitor the time-averaged fluorescent intensity of the atoms as the frequency separation between the two fields is varied. A similar experiment was done in the past in the rf regime.1 For the first time, we report the observation of multiple, well-resolved resonances in the absorption spectrum of the field in the optical regime. We present data and theory for several values of detuning between the fixed field and atomic resonance. The experimental results are in good agreement with theory.