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Laser Physics

Generalized stimulated Raman scattering with nonlocal effects

S Shreyes, Y Huang, C. H. Raymond Ooi

Published Aug 10, 2023• 3 citations
Publisher

Abstract

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.

DOI
10.1088/1555-6611/ace9cf

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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.
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.
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.
A photon theory of the stimulated Raman effect is developed. A system of coupled equations for the amplitudes of scattered photons and molecular vibrations are derived. The molecular vibration coordinates are then eliminated using the random phase approximation. The equations which result assume the form of coupled equations for the first Stokes and anti-Stokes lights. The secular equation which characterizes the solution of these coupled equations is shown to be equivalent to that of Shen and Bloembergen. Using this secular equation, the condition for temporal growth of the scattered lights is obtained and is compared with that for the spatial growth, which was obtained previously by Shen and Bloembergen. It is shown that both types of growth (temporal and spatial) proceed with comparable rates if the damping of the molecular vibration is large. If its damping is small, however, the temporal growth prevails over the spatial growth. Typical line-shape of the anti-Stokes line is obtained in the case of small damping. The result shows a strong directionality, as is the case of large damping.
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.
A quantum theory of stimulated Raman scattering is presented that takes into account three-dimensional propagation and collisional dephasing, allowing the study of the spatial and temporal coherence properties of the generated Stokes light. Maxwell-Bloch equations for the Stokes field operator and the collective atomic operators are solved analytically under low-signal-gain conditions, where the laser field and the atomic ground states remain undepleted. The intensity and the space-time autocorrelation function of the Stokes field are calculated. The Stokes field is expanded into a set of statistically independent ``coherence modes,'' which are determined explicitly for the case of a cylindrically shaped pumped volume. The Stokes pulse energy W is found to fluctuate from pulse to pulse. The probability distribution function for pulse energies P(W) is calculated for a range of Fresnel numbers of the excited volume and collisional dephasing rates. For small values of Fresnel number and dephasing rate, P(W) is a negative exponential distribution. For large values of either, P(W) narrows and approaches a Gaussian-shaped distribution. This occurs because many independent modes contribute to the Stokes emission, making it spatially and/or temporally incoherent.
A theory of stimulated Raman scattering (SRS) is presented which treats in a unified manner the buildup of SRS from spontaneous Raman scattering and the spatial propagation which leads to gain. Maxwell-Bloch equations describe the coupling between the Stokes field operator and the collective atomic operators, which are driven by a classical laser field under low-signal-gain conditions, where the atomic ground states and laser field remain undepleted. An analytic expression is derived for the forward-propagating Stokes field operator in a one-dimensional spatial approximation when the Fresnel number of the excited medium is unity. Steady-state and transient Stokes intensities are evaluated under low-gain (spontaneous) and high-gain (stimulated) conditions. The Stokes intensity is found to be exactly independent of a laser bandwidth arising solely from phase fluctuations. The power spectrum of steady-state SRS is evaluated, giving a gain-narrowed spectral profile when the laser is narrow band, and a spectrum identical to the laser spectrum when the laser is broad band. A strong analogy between SRS and two-level superfluorescence is found; in both cases the macroscopic, collective dipole moment is initiated by quantum fluctuations.