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Quantum Light Scattering in Disordered and Structured Media

Nooshin M. Estakhri

Published Jan 1, 2021• 0 citations
Publisher

Abstract

Understanding the complex interactions of the quantum light with different media provides valuable insights into potential applications in quantum tomography, microscopy, circuit and network design, and imaging. This thesis investigates quantum light interaction with two types of media: I. Random media entailing multiple scattering (Chapters 2-5), and II. Structured media, specifically designed to control quantum interferences (Chapters 6 and 7). In the first part of the thesis, and through solving the Lippmann-Schwinger equation for collections of small scatterers, a first principle scalar model for multiple scattering in finite-sized random media is developed. This efficient numerical model serves as the basis for investigating the coherent backscattering, a manifestation of weak localization in random media, for several bounded random media and various illuminations. Through employing mode expansion, next, the developed model is adapted to a general class of quantum-optical studies and quantum correlations are successfully derived and analyzed in scattering from finite disordered structures as well as systems of few scatterers. In multiple scattering of two-photon states in weak localization regime, the emergence of coherent two-photon backscattering is presented for the first time in coincidence detection, and it is demonstrated that quantum correlations can be used as a probe of entanglement dimensionality. Multiple scattering of two-photon states results in granular patterns known as speckle patterns. The statistical properties of single- and two-photon speckle patterns in scattering of different states are numerically calculated and the speckle visibilities and relevant parameters are derived. Specifically, the deviation of the probability density functions from negative exponential distributions, traditionally recognized as Rayleigh statistics in classical scattering, is identified, and shown to significantly depend on the presence of entanglement. Lastly, a different numerical implementation (based on COMSOL Multiphysics package) is used to consolidate our findings by incorporating the polarization effects. Coherent backscattering and coherent two-photon backscattering are observed for co-polarized fields in scattering from synthesized disordered media. It is demonstrated that depending on the particle exchange symmetry in polarization entangled excitation, the photons can exhibit statistical tendency to bunch together in the same mode, appear in separate modes (antibunching), or show a mixed response after multiple scattering. These bosonic-, fermionic-, and anyonic-like behaviors are studied in connection with coherent backscattering phenomenon, and it is demonstrated that the degree of enhancement in backscattering depends on the exchange symmetries. The simplicity and effectiveness of the implemented scattering analysis and the significance of the consequent conclusions suggest our approach as a promising platform for ‘numerical experiments’ without the limitations of analytical or semi-analytical models, and a practical tool prior to experiments. In the second part of the thesis, the random media operating as multimode platforms are replaced with engineered surfaces, i.e., metasurfaces, to realize targeted quantum interferences. First, a design roadmap for general lossy, asymmetric, and unbalanced coupling networks is presented, allowing to achieve maximum programmability in two-photon interferences. Next, two switchable metasurface-based coupling networks are designed to control nonclassical two-photon interferences via thermally driven crystallographic phase transitions. Numerical simulations confirm smooth transition between coalescence and anti-coalescence, aiming to address the current need in quantum optics for free-space compact devices creating tunable quantum interferences and acting as fast modulators for the second order quantum correlations. Our proposed compact and rapidly controllable devices pave the way towards new quantum applications as well as improving the current free-space quantum systems.

DOI
10.7302/3076

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Understanding the complex interactions of the quantum light with different media provides valuable insights into potential applications in quantum tomography, microscopy, circuit and network design, and imaging. This thesis investigates quantum light interaction with two types of media: I. Random media entailing multiple scattering (Chapters 2-5), and II. Structured media, specifically designed to control quantum interferences (Chapters 6 and 7). In the first part of the thesis, and through solving the Lippmann-Schwinger equation for collections of small scatterers, a first principle scalar model for multiple scattering in finite-sized random media is developed. This efficient numerical model serves as the basis for investigating the coherent backscattering, a manifestation of weak localization in random media, for several bounded random media and various illuminations. Through employing mode expansion, next, the developed model is adapted to a general class of quantum-optical studies and quantum correlations are successfully derived and analyzed in scattering from finite disordered structures as well as systems of few scatterers. In multiple scattering of two-photon states in weak localization regime, the emergence of coherent two-photon backscattering is presented for the first time in coincidence detection, and it is demonstrated that quantum correlations can be used as a probe of entanglement dimensionality. Multiple scattering of two-photon states results in granular patterns known as speckle patterns. The statistical properties of single- and two-photon speckle patterns in scattering of different states are numerically calculated and the speckle visibilities and relevant parameters are derived. Specifically, the deviation of the probability density functions from negative exponential distributions, traditionally recognized as Rayleigh statistics in classical scattering, is identified, and shown to significantly depend on the presence of entanglement. Lastly, a different numerical implementation (based on COMSOL Multiphysics package) is used to consolidate our findings by incorporating the polarization effects. Coherent backscattering and coherent two-photon backscattering are observed for co-polarized fields in scattering from synthesized disordered media. It is demonstrated that depending on the particle exchange symmetry in polarization entangled excitation, the photons can exhibit statistical tendency to bunch together in the same mode, appear in separate modes (antibunching), or show a mixed response after multiple scattering. These bosonic-, fermionic-, and anyonic-like behaviors are studied in connection with coherent backscattering phenomenon, and it is demonstrated that the degree of enhancement in backscattering depends on the exchange symmetries. The simplicity and effectiveness of the implemented scattering analysis and the significance of the consequent conclusions suggest our approach as a promising platform for ‘numerical experiments’ without the limitations of analytical or semi-analytical models, and a practical tool prior to experiments. In the second part of the thesis, the random media operating as multimode platforms are replaced with engineered surfaces, i.e., metasurfaces, to realize targeted quantum interferences. First, a design roadmap for general lossy, asymmetric, and unbalanced coupling networks is presented, allowing to achieve maximum programmability in two-photon interferences. Next, two switchable metasurface-based coupling networks are designed to control nonclassical two-photon interferences via thermally driven crystallographic phase transitions. Numerical simulations confirm smooth transition between coalescence and anti-coalescence, aiming to address the current need in quantum optics for free-space compact devices creating tunable quantum interferences and acting as fast modulators for the second order quantum correlations. Our proposed compact and rapidly controllable devices pave the way towards new quantum applications as well as improving the current free-space quantum systems.
Abstract We present the emergence of coherent two-photon backscattering, a manifestation of weak localization, in multiple scattering of maximally entangled pure and fully mixed two-photon states and examine the effect of entanglement and classical correlations. Quantum correlations in backscattering are investigated for finite three-dimensional disordered structures in the weak localization regime, as well as systems of a small number of scatterers with specified spatial arrangements. No assumptions are made about the statistical behavior of the scattering matrix elements. Furthermore, we study the interplay between quantum correlations induced by multiple scattering and the correlations that may be present in the illumination fields, and how they are manifested in the output modes. We study the effect of the dimensionality of the entanglement and the angular distribution of the jointly measurable photon pairs on the emergence of enhancement and angular quantum correlations and show how quantum correlations can be used as a probe of the entanglement dimensionality. We show that by increasing the disordered material density, the width of the coherent two-photon backscattering cones increases, in accordance with the reduction of the mean free path length within the structure.
This dissertation contains scientific research within the realm of quantum optics, which is a branch of physics. An experimental and theoretical study is made of two-photon interference phenomena in various optical systems. Spatially entangled photon pairs are produced via the nonlinear optical process of spontaneous parametric down-conversion. These entangled photons are then passed through different optical systems to study various aspects of two-photon interference. Firstly, an experimental analysis is made of the high-dimensional entanglement that is present in the orbital angular momentum of the photons. Secondly, we present a comprehensive description of two-photon quantum interference behind a double slit. We demonstrate how to control the quantum correlations and present the first observations of complete two-photon diffraction patterns behind a double slit. Finally, we present pioneering experiments on spatially entangled two-photon states that are scattered of random media. We have observed and theoretically analyzed the structure in the random two-photon interference patterns called two-photon speckle patterns. Spatial entanglement gives two-photon speckle a much richer structure than ordinary one-photon speckle. Our experiments also demonstrate a two-photon interference phenomenon that survives averaging over different realizations of disorder. The latter results are closely related to bosonic, fermionic, and anyonic particle exchange symmetries.
This thesis concerns the theoretical investigation of interference phenomena related to elastic and inelastic scattering of quantized light. The presented work is naturally divided into two parts, the first is concerning elastic scattering while the second explores inelastic scattering. In the first part we use a scattering-matrix formalism combined with results from random-matrix theory to investigate the interference of quantum optical states on a multiple scattering medium. We investigate a single realization of a scattering medium thereby showing that it is possible to create entangled states by interference of squeezed beams. Mixing photon states on the single realization also shows that quantum interference naturally arises by interfering quantum states. We further investigate the ensemble averaged transmission properties of the quantized light and see that the induced quantum interference survives even after disorder averaging. The quantum interference manifests itself through increased photon correlations. Furthermore, the theoretical description of a measurement procedure is presented. In this work we relate the noise power spectrum of the total transmitted or reflected light to the photon correlations after ensemble averaging. This analysis enables us to describe an experimental observation of the quantum nature of light that survives the averaging over disorder. In the second part we investigate inelastic scattering. This we do by first treating the scattering of light on dipoles embedded in an arbitrary dielectric environment. By considering the two different models for dipole interaction known as the minimal-coupling and electric-dipole interaction Hamiltonians, we find exact relations between the electric field and the dipole operators in the Heisenberg picture, while keeping the model of the dipoles arbitrary. Due to the exact treatment of the electric-field operators, we obtain kernels known from classical scattering theory to describe the propagation of the field from the dipoles. Using the found electric field operators we derive the Heisenberg equations of motion for the dipoles while treating them as quantum two-level systems and using the Born–Markov and rotating-wave approximations. Postponing the rotating-wave approximation to the very end of the formal calculations allows us to identify the different physical parameters of the dipole evolution in terms of physical quantities known from optics. Finally, we use our Heisenberg picture formalism to treat a dilute cloud of two-level atoms, by simplifying the equations of motion using a single-scattering approximation for the interaction between the atoms. This enables us to derive expressions for the steady-state population and fluorescence spectrum, where we find cooperative effects in both the elastic and the inelastic spectra.
This thesis presents the author's work on multiple scattering of intense laser light by cold atoms in chapter 2 and nonlinear coherent backscattering in chapter 3. The basic concepts and most important results should be understandable from reading these chapters on their own, whereas we refer to the subsequent collection of articles (P1-P11) for more detailed treatments. In chapter 2.1, we review scattering of light by a single two-level atom, with special emphasis on the fact that the atoms are nonlinear and inelastic scatterers, which will be relevant for multiple scattering. In chapter 2.2, we treat double scattering by two distant atoms, before we generalize this technique to a dilute disordered sample of many atoms in chapter 2.3. Both 2.2 and 2.3 apply in the perturbative regime of low laser intensity, where, by analyzing scattering of two photons, we clarify the different roles of nonlinearity and inelasticity concerning the coherent backscattering interference. Chapter 2.4 discusses the master equation as a complementary approach, applicable at arbitrarily high laser intensity, but only for a small number of atoms. In addition, we present an equivalent new approach, which explicitly takes advantage of the large distance between the atoms, and thereby combines the advantages of the master equation and the scattering approach. As discussed in chapter 2.5, this new approach opens the way to a non-perturbative theory for multiple scattering of intense laser light by dilute atomic clouds. Chapter 3 presents our diagrammatic theory for nonlinear coherent backscattering of classical (or single-particle quantum) waves. In chapter 3.1, we explain the most important assumptions of the theory: weak disorder and small nonlinearity, in particular existence of a stable, stationary solution of the nonlinear wave equation. In chapter 3.2, we explain why - contrary to seemingly convincing intuitive reasoning - the nonlinearity indeed changes the height of the coherent backscattering interference peak. In order to describe this effect quantitatively, a diagrammatic theory is sketched in chapters 3.3 and 3.4, where the nonlinear Born series and the nonlinear ladder and crossed diagrams are introduced. Chapter 3.5 presents the transport equations which result from the complete summation of ladder and crossed diagrams - non-perturbatively in the strength of the nonlinearity. We discuss the conditions under which the nonlinearity reduces or enhances the coherent backscattering interference, as compared to the linear case. In order to confirm the validity of the diagrammatic analysis, we compare these results with numerical simulations in chapter 3.6. We conclude with a short account of our work on speckle instabilities for nonlinear point scatterers in chapter 3.7. Finally, chapter 4 describes some future perspectives of our work, in particular the application of the diagrammatic theory to describe the impact of nonlinearity on weak localization and Anderson localization, and possible extensions to the quantum many-particle regime.
Mesoscale optics provides a framework for understanding a wide range of phenomena occurring in a variety of fields ranging from biological tissues to composite materials and from colloidal physics to fabricated nanostructures. When light interacts with a complex system, the outcome depends significantly on the length and time scales of interaction. Mesoscale optics offers the apparatus necessary for describing specific manifestations of wave phenomena such as interference and phase memory in complex media. In-depth understanding of mesoscale phenomena provides the required quantitative explanations that neither microscopic nor macroscopic models of light-matter interaction can afford. Modeling mesoscopic systems is challenging because the outcome properties can be efficiently modified by controlling the extent and the duration of interactions. In this dissertation, we will first present a brief survey of fundamental concepts, approaches, and techniques specific to fundamental light-matter interaction at mesoscopic scales. Then, we will discuss different regimes of light propagation through randomly inhomogenous media. In particular, a novel description will be introduced to analyze specific aspects of light propagation in dense composites. Moreover, we will present evidence that the wave nature of light can be critical for understanding its propagation in unbounded highly scattering materials. We will show that the perceived diffusion of light is subjected to competing mechanisms of interaction that lead to qualitatively different phases for the light evolution through complex media. In particular, we will discuss implications on the ever elusive localization of light in three-dimensional random media. In addition to fundamental aspects of light-matter interaction at mesoscopic scales, this dissertation will also address the process of designing material structures that provide unique scattering properties. We will demonstrate that multi-material dielectric particles with controlled radial and azimuthal structure can be engineered to modify the extinction cross-section, to control the scattering directivity, and to provide polarization-dependent scattering. We will show that dielectric core-shell structures with similar macroscopic sizes can have both high scattering cross-sections and radically different scattering phase functions. In addition, specific structural design, which breaks the azimuthal symmetry of the spherical particle, can be implemented to control the polarization properties of scattered radiation. Moreover, we will also demonstrate that the power flow around mesoscopic scattering particles can be controlled by modifying their internal heterogeneous structures. Lastly, we will show how the statistical properties of the radiation emerging from mesoscopic systems can be utilized for surface and subsurface diagnostics. In this dissertation, we will demonstrate that the intensity distributions measured in the near-field of composite materials are direct signatures of the scale-dependent morphology, which is determined by variations of the local dielectric function. We will also prove that measuring the extent of spatial coherence in the proximity of two-dimensional interfaces constitutes a rather general method for characterizing the defect density in crystalline materials. Finally, we will show that adjusting the spatial coherence properties of radiation can provide a simple solution for a significant deficiency of near-field microscopy. We will demonstrate experimentally that spurious interference effects can be efficiently eliminated in passive near-field imaging by implementing a random illumination.
We report on the effects of quantum interference induced by the transmission of an arbitrary number of optical quantum states through a multiple-scattering medium. We identify the role of quantum interference on the photon correlations and the degree of continuous variable entanglement between two output modes. It is shown that quantum interference survives averaging over all ensembles of disorder and manifests itself as increased photon correlations due to photon antibunching. Furthermore, the existence of continuous variable entanglement correlations in a volume speckle pattern is predicted. Our results suggest that multiple scattering provides a promising way of coherently interfering many independent quantum states of light of potential use in quantum information processing.