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Journal of Physics B Atomic and Molecular Physics

Time-dependent pulses in quantum optics: the use of Light's perturbation theory

Peter Rodgers, S. Swain

Published Feb 14, 1987• 14 citations
Publisher

Abstract

The problem of a two-level atom interacting with an external, time-dependent field is solved approximately using Light's perturbation theory. The solutions obtained are compared with accurate numerical solutions for three specific time profiles. The agreement is found to be excellent except for a certain range of detunings, and even in this range the agreement is good. The validity of an adiabatic approximation is also assessed.

DOI
10.1088/0022-3700/20/3/022

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The problem of a two-level atom interacting with an external, time-dependent field is solved approximately using Light's perturbation theory. The solutions obtained are compared with accurate numerical solutions for three specific time profiles. The agreement is found to be excellent except for a certain range of detunings, and even in this range the agreement is good. The validity of an adiabatic approximation is also assessed.
The multiple-linear-time-scale method is used to construct a perturbation theory for NNN-level quantum systems subjected to time-dependent perturbations. The secular and small-denominator terms which plague conventional time-dependent perturbation theory are avoided; consequently, the theory is useful for treating long-term behavior and resonant interactions. The introduction of a self-energy operator allows the shifts in energy levels to be displayed explicitly. When the perturbation is the dipole interaction with an electromagnetic field, the successive approximations yield the well-known rotating-wave approximation, corrections due to counter rotating terms, and the Bloch-Siegert frequency shift. The formalism is applicable to arbitrary pulse shapes, provided that $\ensuremath{\parallel}{H}_{1}\ensuremath{\parallel}\ensuremath{\ll}\ensuremath{\hbar}\overline{\ensuremath{\omega}}$, where $\ensuremath{\parallel}{H}_{1}\ensuremath{\parallel}$ represents the inter-action strength and $\overline{\ensuremath{\omega}}$ is a characteristic frequency of the field. Rabi oscillations induced by multiphoton resonances are automatically included, and this effect is demonstrated in the case of a square pulse with frequency approximately one half the resonance frequency for a transition between two vibrational levels of a molecule. These calculations are compared to an exact numerical solution in order to find the limits of validity of the approximation. Even at high intensities ($I\ensuremath{\sim}{10}^{14}$ W/cm2{\mathrm{cm}}^{2}cm2) the shifted resonance frequency is quite accurate; however, the approximate and exact solutions are slightly out of phase, so that the approximate solution can only be trusted for a few Rabi cycles. For much lower intensities ($I\ensuremath{\sim}{10}^{10}$ W/cm2{\mathrm{cm}}^{2}cm2), the approximate solution is valid for many thousands of Rabi cycles.
We derive two types of perturbative approximation for the response of collisionally broadened two-level atoms to a time-dependent field. The perturbative approximations for the inversion and polarization are valid to any desired order in the derivatives of the field. Comparison with a numerical solution of the full density-matrix equations of motion demonstrates that the new approximations significantly improve upon the adiabatic-following and collisional steady-state approximations for time-dependent pulses in the appropriate damping regime. Application of the approximations to pulse propagation, sideband instability, and population pulsations is discussed. The collisional steady-state and adiabatic-following approximations find extensive use in many areas of nonlinear optics. The deficiencies of these approximations are well known: The collisional steady-state approxirnation is valid only for monochromatic (cw) radiation and the adiabatic-following approximation is valid only in the absence of damping and only if the product of the detuning and a characteristic time is much larger than one. In spite of their manifest faults, the collisional steady-state and adiabatic-following approximations are often exceptionally good approximations, in the appropriate damping regime, for the local response of a vapor of two-level atoms to a slowly varying field. However, timedependent nonlinear processes modify a propagating field zuch that it varies less slowly and the neglected portions of the atomic response become more important. ' Therefore improved approximations for the damped atomic response to a time-dependent field are desirable. In this paper we present two improved perturbative approximations for the inversion and polarization of collisionally broadened two-level atoms induced by a time-dependent field. The adiabatic-following approximation for two-level systems was derived phenomenologically by Grischkowsky, who used it to explain certain experimental results of near-resonance laser-pulse propagation. Motivated by the work of Grischkowsky, Crisp provided an analytic derivation for the adiabatic-following approximation and obtained a quadrature for the error. The essential feature of Crisp's derivation is the expansion of the kernel of the integral representation of the off-diagonal density-matrix element p2, in a Fourier series with integration proceeding term by term. Both the adiabatic-following approximation and the collisional steady-state approximation were obtained in first order. Both Crisp and Grischkowsky used the adiabatic inversion to derive a correction to the adiabatic-following approximation for the polarization. We have shown how Crisp's method can be extended to obtain corrections to the adiabatic inversion and to improve corrections to the polarization in the absence of damping. In this paper we show how the integrated Fourier series can be used to obtain two types of perturbative approximation for the inversion and polarization of collisionally broadened twolevel systems that are valid to any desired order in the derivatives of the field. The two types of perturbative approximation to the inversion are (i) a formal solution of the rate equation for the inversion which is obtained from the density-matrix equations for the populations; and (ii) an approximation obtained using the approximation (p22 — p») —I — 4p2, P, 2, valid for weak damping. The approximations for the polarization are obtained by substituting either (i) or (ii) for the inversion in the integrated-Fourier-series expansion of p2, . The approximation obtained using the first type of approximate inversion converges most rapidly for strong damping and reduces to the collisional steady-state approximation when the magnitude and phase of the field are constant. The approximation obtained using the second type of approxirnate inversion converges most rapidly for weak damping and in first order reduces to the adiabaticfollowing approximation for zero damping. Comparison with a numerical solution of the density-matrix equations demonstrates that retention of higher-order derivatives by retaining more terms in the integrated Fourier series results in a significant improvement in accuracy for a time-dependent field. However, Rabi oscillations, which can be an important component of the nonlinear response, ' cannot be obtained by finite-order approxi
A time-dependent perturbation theory for the solution of the time-dependent Schrödinger equation is developed and is applied to systems having two states with pulse and Lorentzian types of perturbations. It is shown in the case of the pulse perturbation that the expression corresponding to the Nth order of the perturbation theory converges to the exact solution when N tends to infinity. The results obtained from this perturbation theory, the Magnus approximation, and the time-dependent perturbation theory developed by Dirac are compared with the exact results. This theory is found to be good for larger values of the perturbations and for larger intervals of time.
We derive two types of perturbative approximation for the response of collisionally broadened two-level atoms to a time-dependent field. The perturbative approximations for the inversion and polarization are valid to any desired order in the derivatives of the field. Comparison with a numerical solution of the full density-matrix equations of motion demonstrates that the new approximations significantly improve upon the adiabatic-following and collisional steady-state approximations for time-dependent pulses in the appropriate damping regime. Application of the approximations to pulse propagation, sideband instability, and population pulsations is discussed.
Adiabatic Approximation in Interaction Between Two-Level Atom in an External Potential Vx^V{\hat x}Vx^ and Optical Field