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Proceedings of SPIE, the International Society for Optical Engineering/Proceedings of SPIE

Photon statistics: classical and quantum fluctuations of scattered light in an optical anisotropic (ordered) liquid

Sergei M Arakelyan

Published Jun 17, 1993• 0 citations
Publisher

Abstract

The brief review of experimental results on the light scattering (both linear and nonlinear) in liquid crystals in critical range, which have been obtained by the original homodyne technique, is presented. The multiplicative nature of the molecular fluctuations in the medium under external field and physical consequences of that are discussed.

DOI
10.1117/12.146213

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The brief review of experimental results on the light scattering (both linear and nonlinear) in liquid crystals in critical range, which have been obtained by the original homodyne technique, is presented. The multiplicative nature of the molecular fluctuations in the medium under external field and physical consequences of that are discussed.
Laser-induced bulk gratings and temporal instabilities of nonlinear wave processes with different components of light polarization have been studied in the liquid crystals (LC). A mirrorless feedback arises because of the non-local nonlinear response of an anisotropic elastic medium on the external field. The multiplicative nature of the molecular fluctuations in the LC under external field are discussed and the light-induced reorientation effects in this medium can be considered as a noise-induced phase transition. . The quantum aspects of behavior of the radiation fluctuations for passing through the LC light are considered. A new method of formation of quantum states of the light in the linear system at dynamic diffraction is discussed for the first time. The squeezed states of the field and the photon superbunching are obtained for two geometries (Bragg and Laue) of diffraction in spatially periodic medium. The approach gives a new opportunities for a verification of quantum properties of the light in experiment.
A review is given of experimental and theoretical achievements in studies of multiphoton spontaneous scattering processes in atomic and molecular media. An analysis is made of integral multiphoton scattering, particularly of scattering in statistically inhomogeneous media with short-range quasiorder. A study of the intensity of the noncoherent multiphoton scattering component provides direct information on the nonlinear polarizability of atoms and molecules whilst the coherent component is associated with various atomic and molecular correlation mechanisms. An analysis of the spectra of elastic and inelastic multiphoton scattering processes yields information on the translational and rotational motion of the molecules. In particular, it is possible to measure the higher-order rotational relaxation times and to verify the adequacy of the various stochastic models of molecular motion. Observations of the spectral lines of three- or more-photon scattering, which obeys new selection rules, yield detail on the fine structure of the molecules and their linear and nonlinear vibrations. Examples are given of the most interesting spectra of three- or more-photon scattering in gases, liquids, and crystals obtained in singleand multichannel systems. The stochastic theory of multiphoton scattering in liquids is discussed, using the spherical tensor concept. The derived general expression reduces to known results for certain cases.
The physical aspects of the manifestation of optical bistability, instabilities, and stochasticity in strongly nonlinear media in the form of liquid crystals subjected to laser radiation fields are discussed. The stress is on experimental research. Optical bistability and multistability are considered for a number of light-induced effects in homogeneous and inhomogeneous liquid crystals. The special features of these effects in liquids crystals, associated with the field-induced structural phase transitions, are stressed and the concept of intrinsic (mirrorless) optical bistability is introduced. General nonlinear systems with optical bistability are considered. An analysis is made of instabilities and stochasticity manifested in experiments on light-induced reorientation of liquid crystals in the presence of fields of different origin, giving rise to oscillatory and chaotic processes in the case of self-modulation of the transmitted light.
The theory of optical birefringence is discussed from the point of view of the scattering of polarized photons by molecules using the framework of formal scattering theory and quantum electrodynamics. In Part One, those features from noncovariant quantum electrodynamics relevant to the molecular scattering of photons are reviewed. Chapter One contains an outline of classical electrodynamics in the Coulomb gauge, including the Stokes parameter and density matrix formulations of polarization. Chapter Two deals with the quantization of the radiation field, and the occupation number representation is defined. The quantum mechanical description of polarized light is outlined in Chapter Three: operator equivalents of the density matrix and Stokes parameters are invoked, the parameters themselves being obtained from the expectation values of the Stokes operators with the state vector of the photon. The Stokes parameter and density matrix are then applied to the polarization of a general beam containing an arbitrary number of photons, and some new methods are developed. The interaction of the electromagnetic field with bound electrons is formulated in Chapter Four in terms of a canonically transformed interaction Hamiltonian in which the multipole terms are explicit. Since each term is then gauge-invariant, this Hamiltonian is particularly suited to the application of diagrammatic perturbation theory which follows from the iteration of the scattering matrix in the interaction representation (Chapter Five). Also the extension of the theory to multiphoton processes is facilitated "because the field strength is explicit in the transformed Hamiltonian. The S-matrix connects the initial and final asymptotic states of the scattering system, and in Chapter Six the state vector and density operator of the scattered photon beam are obtained from those of the incident beam. Part Two contains the application of the above methods to a variety of linear and nonlinear optical birefringence effects in the absence or presence of external fields. In Chapter Seven, general equations are obtained for the polarization changes imposed on a forward scattered photon in terms of matrix elements of the reaction operator between plane polarized photon base states; whereas Chapter Eight extends this treatment to an n-photon beam, thereby encompassing the hyperpolarizability contributions to the polarization changes of the forward scattered beam. It is then demonstrated that the fundamental process in optical birefringence can be interpreted as an infinitesimal unitary transformation of the polarization spinor. Also the S-matrix approach to birefringence is compared with the methods used in crystal optics, and with the classical treatments of the scattering of polarized light by molecules. The general equations obtained for the polarization changes of the forward scattered beam are subsequently interpreted in the light of the physical circumstances appropriate to the bire- fringence effect of interest. In Chapters Nine, Ten, and Eleven, diagrammatic perturbation theory is used to obtain explicit expressions, in terms of molecular polarizability and rotation tensors, for the linear and nonlinear contributions to the polarization changes involved in natural optical activity, and in birefringence phenomena induced by static and optical electric and magnetic fields. The nonforward scattering of polarized photons by molecules is discussed in Part Three. General equations are calculated in Chapter Twelve for the azimuth, ellipticity, and depolarization ratio of the Rayleigh beam at any scattering angle and for any polarization of the incident beam. Explicit expressions in terms of molecular quantities are then obtained for the polarization at scattering angles of 90° and almost zero from both optically inactive and optically active molecules. It is demonstrated that a determination of the precise polarization state of the scattered beam can provide useful molecular information additional to that obtained from depolarization ratios alone. This is because the depolarization ratio depends on only the diagonal elements of the polarization density matrix and so does not convey all the information about the system. Raman scattering processes are contained in the formulation and the polarization of the Raman light at any scattering angle can be obtained. This is shown to be particularly useful for predicting the polarization of stimulated Raman light for any Raman-active liquid placed within a laser cavity. By extending the nonforward scattering formulation to incorporate multiphoton processes, equations are obtained in Chapter Thirteen for the ellipticity, azimuth, and depolarization ratio of the second harmonic wave at any scattering angle as a function of the incident polarization. Several specific situations are subsequently investigated. Finally, it is shown in Chapter Fourteen that the near-forw- ard Rayleigh and Raman scattering formulations provide an explanation for the observed polarization, as a function of the initial polarization, of the self-trapped filaments that arise from the self-focusing of an intense laser beam.
Structural disorder results in multiple scattering in real photonic crystals, which have been widely used for applications and studied for fundamental interests. The interaction of light with such complex photonic media is expected to show interplay between disorder and order. For a completely disordered medium, the intensity statistics is well-known to obey Rayleigh statistics with a negative exponential distribution function, corresponding to absence of correlations. Intensity statistics is unexplored however for complex media with both order and disorder. We study experimentally the intensity statistics of light reflected from photonic crystals with various degree of disorder. We observe deviations from the Rayleigh distribution and the deviations increase with increasing long-range order.