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Scientific Reports

Time-ordering in Heisenberg’s equation of motion as related to spontaneous radiation

Benjamin D. Strycker

Published Nov 12, 2021• 1 citation
Publisher

Abstract

Despite many years of research into Raman phenomena, the problem of how to include both spontaneous and stimulated Raman scattering into a unified set of partial differential equations persists. The issue is solved by formulating the quantum dynamics in the Heisenberg picture with a rigorous accounting for both time- and normal-ordering of the operators. It is shown how this can be done in a simple, straightforward way. Firstly, the technique is applied to a two-level Raman system, and comparison of analytical and numerical results verifies the approach. A connection to a fully time-dependent Langevin operator method is made for the spontaneous initiation of stimulated Raman scattering. Secondly, the technique is demonstrated for the much-studied two-level atom both in vacuum and in a lossy dielectric medium. It is shown to be fully consistent with accepted theories: using the rotating wave approximation, the Einstein A coefficient for the rate of spontaneous emission from a two-level atom can be derived in a manner parallel to the Weisskopf-Wigner approximation. The Lamb frequency shift is also calculated. It is shown throughout that field operators corresponding to spontaneous radiative terms do not commute with atomic/molecular operators. The approach may prove useful in many areas, including modeling the propagation of next-generation high-energy, high-intensity ultrafast laser pulses as well as spontaneous radiative processes in lossy media.

DOI
10.1038/s41598-021-01781-7

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Despite many years of research into Raman phenomena, the problem of how to include both spontaneous and stimulated Raman scattering into a unified set of partial differential equations persists. The issue is solved by formulating the quantum dynamics in the Heisenberg picture with a rigorous accounting for both time- and normal-ordering of the operators. It is shown how this can be done in a simple, straightforward way. Firstly, the technique is applied to a two-level Raman system, and comparison of analytical and numerical results verifies the approach. A connection to a fully time-dependent Langevin operator method is made for the spontaneous initiation of stimulated Raman scattering. Secondly, the technique is demonstrated for the much-studied two-level atom both in vacuum and in a lossy dielectric medium. It is shown to be fully consistent with accepted theories: using the rotating wave approximation, the Einstein A coefficient for the rate of spontaneous emission from a two-level atom can be derived in a manner parallel to the Weisskopf-Wigner approximation. The Lamb frequency shift is also calculated. It is shown throughout that field operators corresponding to spontaneous radiative terms do not commute with atomic/molecular operators. The approach may prove useful in many areas, including modeling the propagation of next-generation high-energy, high-intensity ultrafast laser pulses as well as spontaneous radiative processes in lossy media.
In the master equation method, we have already illustrated a powerful technique for the calculation of the dynamics of an atomic system interacting with the vacuum field. Another technique for calculating the dynamics of an atomic system coupled to the elec- tromagnetic (EM) field involves Heisenberg equations of motion for the system’s operators. A difference between the master equation and the Heisenberg equations is that the later involves dynamics of the operators, which allows to analyse the evolution of an atomic system in terms of the field and atomic operators. This creates some problems with handling the Heisenberg equations as, in general, operators do not commute and then in the course of solution of the equations we may face the problem of ordering of the operators. It is usually resolved by putting the operators in the normal order. We have gained some experience with the Heisenberg equations of motion in Chapter 6, Example 6.3, where we studied squeezing generation in the nonlinear degenerate parametric amplifier (DPA) process. Here, we illustrate the technique on the standard model of a two-level atom interacting with a multi-mode field. We then generalize the technique to some specific models such as Lorenz- Maxwell and Langevin equations, the derivation of which involves some approximations that can be applied only in some limited cases. We also present in detail the Floquet approach, which is usually applied to problems determined by differential equations with time- dependent coefficients.
Abstract We present a generalized quantum theory of stimulated Raman scattering, which is based on coupled Heisenberg–Langevin equations. Analytical solutions in previous models neglect the effects of the frequency dispersion, assume far-off resonance and only consider slowly varying terms in the atomic operator. In obtaining the more general theory, we have derived partial integro-differential equation containing polarization kernels that include all the temporal nonlocal effects using systematic integral method over time. Analytical solutions of the Stokes field with greater generality for arbitrary spatial-temporal laser fields have been obtained using Laplace transform in the retarded space frame with minimal approximations made. The solutions are very general and potentially useful for studying systems in which highly accurate modeling is required such as quantum memories of a wide range of Raman systems.
A quantum theory of stimulated Raman scattering is established that takes into account the time-dependence of pump laser pulse, two-photon detuning and atomic populations, allowing the general transient and spatial propagation study of Raman memory. Heisenberg–Langevin and Maxwell equations for the collective atomic operators are solved analytically under adiabatic condition , where the electric field envelopes and the collective atomic operators vary slowly. The analytical solution of Stokes/anti-Stokes signal electric field operator is obtained. The spatial–temporal intensity of quantum signal field is studied numerically and analytically for different two-photon detunings and initial populations.
The effect of spontaneous decay on the linear polarizability of an atom is typically included by adding imaginary parts to the frequency denominators that appear in the Kramers-Heisenberg formula. It has been shown for a two-level atom with radiative broadening that these (frequency-dependent) imaginary parts must be included in both the resonant and antiresonant frequency denominators [P. W. Milonni and R. W. Boyd, Phys. Rev. A 69, 023814 (2004)]; however, the expression obtained by Milonni and Boyd for the polarizability does not satisfy the optical theorem, if contributions from non-rotating-wave terms are included. In this paper, we derive a more accurate expression for the polarizability. The calculations are rather complicated and require that we go beyond the standard Weisskopf-Wigner approximation. We present calculations carried out in both the Heisenberg and Schr\"odinger pictures, since they offer complementary methods for understanding the dynamics of the Rayleigh scattering associated with the atomic polarizability. Moreover, it is shown that the shifts associated with the excited state are not the Lamb shifts of an isolated atom, but depend on the dynamics of the atom-field interaction. Our results for the polarizability are consistent with those obtained recently by Loudon and Barnett using a Green's-function approach.
Generalized single-atom Maxwell-Bloch equations for optically dense media are derived taking into account noncooperative radiative atom-atom interactions. Applying a Gaussian approximation and formally eliminating the degrees of freedom of the quantized radiation field and of all but a probe atom leads to an effective time-evolution operator for the probe atom. The mean coherent amplitude of the local field seen by the atom is shown to be given by the classical Lorentz-Lorenz relation. The second-order correlations of the field lead to terms that describe relaxation or pump processes and level shifts due to multiple scattering or reabsorption of spontaneously emitted photons. In the Markov limit a nonlinear and nonlocal single-atom density matrix equation is derived. To illustrate the effects of the quantum corrections, we discuss amplified spontaneous emission and radiation trapping in a dense ensemble of initially inverted two-level atoms and the effects of radiative interactions on intrinsic optical bistability in coherently driven systems.
Abstract Stimulated Raman scattering (SRS) is highly relevant to quantum memories involving Raman system. Using quantum Langevin equations with complete noise operators coupled to the quantum field propagation equation, we present a general theory of SRS for moving quantum particles where quantum Stokes pulse couples to both transitions (m1 and m3) while an arbitrary laser pulses couple to only one (m1) transition. Our coupled equations contain dynamical ac Stark shift due to laser pulses and Doppler shift, complete quantum noise operators and atomic coherences corresponding to all possible three transitions (not only the ground state coherence), quantum mechanical microscopic expressions for linear and nonlinear interactions with nonlocal (memory) or temporal dispersion effects. We obtain an analytical solution of the quantum Stokes field in laboratory spacetime with generalized quantum noise operators that include all initial atomic coherences and arbitrary initial and boundary quantum fields, valid for arbitrary laser pulses. The general solution provides a complete physical picture, composed of basically two parts: above and below the light line, t = z/c. This robust framework offers a powerful tool for optimizing Raman-based quantum information processes, particularly for modeling the spatial-temporal dynamics of quantum Stokes pulses in storage and retrieval stages of quantum memory.