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The Journal of Chemical Physics

Nonlinear optical response of three-level systems

Raanan Bavli, Donald F. Heller, Y. B. Band

Published Dec 1, 1989• 20 citations
Publisher

Abstract

We investigate the properties of a homogeneously broadened three-level system interacting with two optical fields, Eω1(x,t) and Eω2(x,t), with central frequencies ω1 and ω2 whose amplitudes are assumed to be slowly varying in time compared with dephasing times of the optical transitions. We calculate Raman susceptibilities allowing each transition to be induced by both fields and without employing the rotating wave approximation (RWA); this enables correct calculation of the optical response of the medium when the fields are on-resonance or arbitrarily far off-resonance with the Raman transition. In some frequency regions the RWA causes substantial errors. A distinction is drawn between two different types of RWA: (a) a neglect of off-resonant components of the polarization for direct optical transitions, and (b) neglect of off-resonant components of off-diagonal density matrix elements of order Eω1(x,t)Eω2(x,t)* in the field amplitudes. The first RWA is known to become inaccurate when the pump frequency is significantly off-resonance with the pump transition. We show that the second RWA becomes inaccurate when ‖ω1−ω2‖ is small or comparable to the active Raman mode frequency (even when the field are close to resonance). Calculations based upon our expressions show that when the pump frequency is close to resonance with the optical transition from the ground state, a nonlinear absorption at the Stokes shifted frequency occurs. This absorption can significantly decrease the Raman gain. Also, we find that Rabi splittings in a three-level system can occur even when the pulse durations of the incident fields are short compared with the T1 times of the system. We solve analytically for the optical response of the system to two fields of arbitrary strength and frequency. We analyze this solution and its perturbative expansion in the field amplitudes. We use the Maxwell–Bloch equations developed here to propagate time-dependent pulses.

DOI
10.1063/1.457339

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We investigate the properties of a homogeneously broadened three-level system interacting with two optical fields, Eω1(x,t) and Eω2(x,t), with central frequencies ω1 and ω2 whose amplitudes are assumed to be slowly varying in time compared with dephasing times of the optical transitions. We calculate Raman susceptibilities allowing each transition to be induced by both fields and without employing the rotating wave approximation (RWA); this enables correct calculation of the optical response of the medium when the fields are on-resonance or arbitrarily far off-resonance with the Raman transition. In some frequency regions the RWA causes substantial errors. A distinction is drawn between two different types of RWA: (a) a neglect of off-resonant components of the polarization for direct optical transitions, and (b) neglect of off-resonant components of off-diagonal density matrix elements of order Eω1(x,t)Eω2(x,t)* in the field amplitudes. The first RWA is known to become inaccurate when the pump frequency is significantly off-resonance with the pump transition. We show that the second RWA becomes inaccurate when ‖ω1−ω2‖ is small or comparable to the active Raman mode frequency (even when the field are close to resonance). Calculations based upon our expressions show that when the pump frequency is close to resonance with the optical transition from the ground state, a nonlinear absorption at the Stokes shifted frequency occurs. This absorption can significantly decrease the Raman gain. Also, we find that Rabi splittings in a three-level system can occur even when the pulse durations of the incident fields are short compared with the T1 times of the system. We solve analytically for the optical response of the system to two fields of arbitrary strength and frequency. We analyze this solution and its perturbative expansion in the field amplitudes. We use the Maxwell–Bloch equations developed here to propagate time-dependent pulses.
The rate of absorption and emission of radiation is calculated for two laser fields interacting with a homogeneously broadened, three-level molecular system. The time-dependent Schrödinger equation is used in the density matrix formalism and the laser fields are treated classically. The laser fields, at frequencies ωpand ωs, are off resonance by δpand δs, respectively, such that|\delta_{p}|, |\delta_{s}| \ll \omega_{p}, \omega_{s}. Analytic expressions are derived for the imaginary part of the electric susceptibility,\chi"(\omega_{p})and\chi"(\omega_{s}). The present work differs from previous calculations in that the laser fields may have arbitrary values of field strength and each field may be on or off resonance. A discussion is presented of the properties of the solutions for\chi"(\omega_{p})and\chi"(\omega_{s}), for both strong and weak laser fields, based on computer evaluation of the general analytic expressions. It is shown that the solutions may be divided into single-photon and two-photon, or Raman, contributions. Conditions for optimizingdI(\omega_{s})/dzand the photon conversion efficiency are derived. These results may be applied to analyzing the pulsed, optically pumped submillimeter laser and to studying two-photon absorption in a gas.
In the domain of semiclassical formulation and for the Doppler-free atom–field interaction, we construct the optical Bloch equations involving an M-type six-level system coupled to two pump fields and a probe field. The response of the system is probed for different pump-induced transitions in double and triple-resonance situations. In order to obtain the coherent lineshapes (absorptive and dispersive), we use the usual perturbation method for obtaining the approximate analytical solutions to these coupled optical Bloch equations for the density matrix elements. The interferences between the probability amplitudes for different energy levels (dipole allowed and dipole forbidden) are taken care of. For off-resonance pump positions, the linewidths of the three probe transitions are insensitive to the pump Rabi frequencies. On the other hand, the shifts of the three resonance peaks are extremely sensitive to the pump Rabi frequencies. However, for on-resonance pump conditions, the sensitivities of pump Rabi frequencies on the linewidths of the resonance peaks and on the shifts of the resonance peak positions are opposite to those of their off-resonance counterparts. In particular, we have shown the asymmetric and symmetric Rabi splittings under different physical conditions, for non-zero and near-zero probe detuning, respectively. The Rabi splitting under triple-resonance conditions, significantly, modifies the dispersive lineshape at the centre of the absorption line. The two- and three-photon absorptions are also reported for different off-resonant pump positions.
We study unidirectional three-wave spectroscopy for which one pump and two probe waves beat in a nonlinear medium at the frequencies ±Δ with respect to the pump. Field transmission spectra change as the fields propagate through the medium due to probe variations in both amplitude and phase. In a homogeneously broadened two-level system, the rates of change in sidemode amplitudes and phases are determined by the effectiveness of the population pulsations in coupling the fields. For cases in which the population difference lifetime T1 is comparable with the dipole lifetime T2, the strong coupling between the sidemodes and the pump leads to fast amplitude change, while strong coupling between the two sidemodes leads to fast phase change. When the pump Rabi flopping frequency Ω ≅ Δ and Δ ≅ 1/T1, the population pulsations couple the two sidemodes most efficiently, causing the sidemode phases relative to the pump phase to vary rapidly. When Ω ≅ 2Δ, the pump field scatters strongly off the population pulsations, thereby amplifying the sidemode fields. When Ω ≫ Δ, the population pulsations become too weak to couple the fields significantly, and phase, amplitude, and spectral features in general change very slowly.
We investigate the interaction of a multilevel atom with a short femtosecond optical pulse beyond the scope of the rotating-wave approximation. We consider the behavior of a three-level atom under the action of two optical pulses resonant with two allowed transitions and a two-level atom under the action of a resonant optical pulse. It is shown that the imaginary part of the off-diagonal elements of the density matrix oscillates with high frequency due to the counter-rotating terms. It is shown also that an effective time-dependent addition to the Rabi frequency exists, which is of importance for ultrashort optical pulses.
We calculate analytically the error introduced by the rotating-wave approximation (RWA) to the description of a two-level-atom response to a resonant sufficiently intense femtosecond optical pulse of a few-cycle duration and any envelope. The analytically calculated non-RWA refinements to the RWA response are of the lowest order, i.e., linear in the small ratio of the Rabi to optical frequencies. One type of such refinements is small-amplitude rapid oscillations at nearly twice the optical frequency superimposed on the standard RWA population-inversion evolution. The other refinement is an extension of the spectrum of the induced atomic dipole moment in which the third harmonic of the transition frequency appears. The spectrum of this harmonic has an internal structure dependent on both strength and duration of the pulse. The analytically found non-RWA corrections are in qualitative agreement with the recent results of different numerical approaches by other authors and a recent experiment.
A theory is presented of induced Raman emission in a three-level system whose parameters are appropriate for microwave to optical frequencies. Solutions of the time-dependent Schrödinger equation are obtained for arbitrary intensity of the pump and signal radiations, which are assumed to be not too many line-widths off resonance. It is shown how the quantum-mechanical aspects of the problem may be separated from the statistical-mechanical aspects, in contrast to the density matrix techniques. The frequency dependence of the Raman emission on the frequency and intensity of the pumping radiation obtained by this method is presented and compared with the results we have obtained by other methods. The intensity and line shape of the Raman emission when the pump frequency is far off resonance are also obtained. The case of three interacting fields is also considered.