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Journal of Modern Optics

Quantum Theory of Hyper-Raman Scattering

Yu. P. Malakyan

Published Mar 1, 1992• 6 citations
Publisher

Abstract

We develop the quantum theory of stimulated hyper-Raman scattering (HRS) and discuss the quantum statistics of pump and Stokes fields. We show that the initially coherent pump field acquires a strong squeezing that exceeds the similar squeezing in other nonlinear processes also involving two-photon absorption. Stokes field statistics are analysed in detail as a function of the initial statistics of both modes. Bunching effects are shown to be amplified in the short-time region, while in asymptotics the antibunching of Stokes photons becomes dominant, which in many cases results in sub-Poissonian statistics of Stokes mode. We also find a number of correlation effects between the photons of the two modes.

DOI
10.1080/09500349214550501

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We develop the quantum theory of stimulated hyper-Raman scattering (HRS) and discuss the quantum statistics of pump and Stokes fields. We show that the initially coherent pump field acquires a strong squeezing that exceeds the similar squeezing in other nonlinear processes also involving two-photon absorption. Stokes field statistics are analysed in detail as a function of the initial statistics of both modes. Bunching effects are shown to be amplified in the short-time region, while in asymptotics the antibunching of Stokes photons becomes dominant, which in many cases results in sub-Poissonian statistics of Stokes mode. We also find a number of correlation effects between the photons of the two modes.
Using the approximation of small fluctuations around a stationary solution, photon statistics and quadrature variances are derived in stimulated Raman and hyper-Raman scattering including the coupling of pumping, Stokes, anti-Stokes and phonon modes. The depletion of pump light is included. Compared to Raman scattering, additional regimes to generate anti-bunched, sub-Poisson and squeezed light were found caused by self-interaction of the pump mode. It was possible to include effects of nonlinear dynamics, initial squeezing of radiation and phonon system, external noise and losses.
The non-classical effects of squeezing of light in coherent anti-Stokes Raman scattering (CARS) and coherent anti-Stokes hyper-Raman scattering (CAHRS) are investigated under the short-time approximation based on a fully quantum mechanical approach. In an idealized model CARS, the interaction is looked upon as a process involving absorption of a pump photon and emission of a Stokes photon, which is followed by absorption of a pump photon and subsequently emission of an anti-Stokes photon at a different frequency, whereas CAHRS is looked upon as a process involving absorption of two pump photons and emission of a Stokes photon, which is followed by absorption of two more pump photons and subsequent emission of an anti-Stokes photon at a different frequency. The coupled Heisenberg equations of motion involving real and imaginary parts of the quadrature operators are established. It is shown that squeezing in the Stokes and anti-Stokes mode in CARS is found to be dependent on amplitude-squared squeezing of the initial pump field while, in CAHRS, it is dependent on the fourth-order amplitude squeezing of the initial pump field. Higher-order squeezing can be converted to linear squeezing through these processes. It is also shown that squeezing is greater in CAHRS than the corresponding squeezing in CARS.
An initially prepared coherent state coupled to a second-order nonlinear medium is responsible for stimulated and spontaneous hyper Raman processes. By using an intuitive approach based on perturbation theory, the Hamiltonian corresponding to the hyper Raman processes is analytically solved to obtain the temporal development of the field operators. It is true that these analytical solutions are valid for small coupling constants. However, the interesting part is that these solutions are valid for reasonably large time. Hence, the present analytical solutions are quite general and are fresh compared to those solutions under short-time approximations. By exploiting the analytical solutions of field operators for various modes, we investigate the squeezing, photon antibunching and nonclassical photon statistics for pure modes of the input coherent light responsible for hyper Raman processes. At least in one instance (stimulated hyper Raman processes for vibration phonon mode), we report the simultaneous appearance of classical (photon bunching) and nonclassical (squeezing) effects of the radiation field responsible for hyper Raman processes.
The nonclassical effect of squeezing of light in hyper-Raman processes is investigated under the short-time approximation based on a fully quantum mechanical approach. Effects of squeezing in spontaneous and stimulated processes are studied. A hyper-Raman process is looked upon as a three-photon and one-phonon interaction process. Squeezing in amplitude, squared amplitude and cubed amplitude have been investigated. Squeezing occurs invariably in the fundamental mode in both spontaneous and stimulated processes, whereas the squeezing in the Stokes mode is found to be dependent on amplitude-squared squeezing of the initial pump field.
Photon statistics of stimulated Raman scattering and degenerate hyper-Raman scattering in the cavity are investigated using the method of small operator corrections to a c-number solution. Weak non-classical effects and super-Poissonian behaviour of all modes are derived in the case of Raman scattering in stationary regime. Higher-order nonlinearity of hyper-Raman scattering leads to more significant non-classical effects—considerable quadrature squeezing and sub-Poissonian behaviour of laser and Stokes modes (Fano factor lower than 0·8) were obtained. A negative quantum noise component is manifested in oscillations of photon-number distribution and in negative values of Wigner distribution of the integrated intensity. The influence of external driving amplitude and thermal bath is examined.
This paper aims to study the photons antibunching in the fundamental, Stokes and signal modes of CAHRS (coherent anti-Stokes hyper Raman scattering). The generalized interaction Hamiltonian was calculated for different conditions in the Heisenberg picture under short time approximation to observe photons antibunching in the fundamental, Stokes and signal modes of CAHRS. It has been found that antibunching in the fundamental field is dependent upon interaction time, photons number, and coupling strength of field. Third order photon antibunching is found to be nonclassical to a greater extent than second- and first-order photon antibunching for the identical pump photons count. It has been also observed that the effect of photon antibunching in Stokes and signal modes is less prominent than in the fundamental- mode. Furthermore, it is also found that antibunching will increase at short interaction timeswith the increase of depth of nonclassical behavior. Finally, the extent of photons antibunching peaks precisely where the second correlation function is lowest.