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arXiv:1803.06191 · Physical Review A

Photon echoes in strongly scattering media: A diagrammatic approach

Romain Pierrat, Rémi Carminati, J.-L. Le Gouët

Published Jun 11, 2018• 2 citations
arXivHTMLPDF

Abstract

We study photon echo generation in disordered media with the help of multiple scattering theory based on diagrammatic approach and numerical simulations. We show that a strong correlation exists between the driving fields at the origin of the echo and the echo beam. Opening the way to a better understanding of nonlinear wave propagation in complex materials, this work supports recent experimental results with applications to the measurement of the optical dipole lifetime ${T}_{2}$ in powders.

DOI
10.1103/physreva.97.063816

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Emission of photon echoes in a strongly scattering medium

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We observe the two- and three-pulse photon echo emission from a scattering powder, obtained by grinding a Pr3+:Y2SiO5 rare earth doped single crystal. We show that the collective emission is coherently constructed over several grains. A well defined atomic coherence can therefore be created between randomly placed particles. Observation of photon echo on powders as opposed to bulk materials opens the way to faster material development. More generally, time-domain resonant four-wave mixing offers an attractive approach to investigate coherent propagation in scattering media.

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Superradiant Damping Effects in Photon-Echo Theory

Antonio M. Ponte Goncalves, Andree A. Tallet, R. Lefèbvre

A theoretical model for superradiant damping effect in inhomogeneously broadened media and its application to photon-echo problems are discussed. Only optically thin systems are considered, and all nonradiative relaxation mechanisms are neglected. Numerical calculations are performed for a very wide square inhomogeneous line shape and square applied pulses. It is shown that excitation of the system becomes increasingly difficult as the superradiant lifetime ${\ensuremath{\tau}}_{s}$ becomes comparable with ${T}_{2}^{*}$. The energy reradiated after the end of the exciting pulse is considerable for ${\ensuremath{\tau}}_{s}\ensuremath{\approx}{T}_{2}^{*}$ and for some applied pulse areas. Two-pulse sequences produce multiple echoes as the microscopic polarizations spontaneously rephase. The first-echo amplitude maximum is found to occur for first-applied-pulse areas increasingly above $\frac{1}{2}\ensuremath{\pi}$ as ${\ensuremath{\tau}}_{s}$ decreases. For a given first-pulse area, the echo intensities increase initially as ${\ensuremath{\tau}}_{s}$ decreases (negligible damping) and finally decrease and vanish (important damping). The ratio of the second- to first-echo amplitudes is found to be proportional to $\frac{{T}_{2}^{*}}{{\ensuremath{\tau}}_{s}}$ for small superradiance levels and to decrease when ${\ensuremath{\tau}}_{s}$ approaches ${T}_{2}^{*}$. An approximate estimate of this ratio is derived for the region of linearity in $\frac{{T}_{2}^{*}}{{\ensuremath{\tau}}_{s}}$.

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The active use of resonators in quantum technologies increases the interest of their application in the creation of optical and microwave quantum memory. The use of photon and spin echoes opens up the possibility of storing a large number of light pulses in one such memory cell. High efficiency of such quantum memory is achieved in an optically dense resonant media, in which the formation of a photon (spin) echo can be accompanied by an increase in the nonlinear interaction of light with atoms causing the appearance of multiple echo signals. In this paper, we develop the pulse area approach to study general nonlinear properties of the primary and multi-pulse echo signals excited in a two-level atomic ensemble located in ring cavities with volumetric and surface modes. Conditions under which one or more echo pulses can be generated are analyzed. The solutions obtained are compared with recent experimental results. We show that the area theorem is one of the simplest and most powerful analytical tools for studying a highly nonlinear and dynamical process of the formation of the sequence of photon/spin echo signals in resonant media inside the resonator.

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Quantum Light Scattering in Disordered and Structured Media

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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.

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The authors derive analytical expressions for secondary echoes formed under the two-pulse excitation of the optically dense media developing McCall-Hahn area theorem for echo effects. They find that a series of self-reviving echo signals with a total area of 2$\ensuremath{\pi}$ or 0$\ensuremath{\pi}$ is excited and propagates deep in the media demonstrating strong non-linear nature of light-matter interaction at small changes of second pulse area. The pulse area approach paves the way for precise coherent spectroscopy, the study of different photon echoes and quantum control of light pulses in the optically dense media.

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Laser Physics•Oct 25, 2019•7 citations
We study photon echo generation in disordered media with the help of multiple scattering theory based on diagrammatic approach and numerical simulations. We show that a strong correlation exists between the driving fields at the origin of the echo and the echo beam. Opening the way to a better understanding of nonlinear wave propagation in complex materials, this work supports recent experimental results with applications to the measurement of the optical dipole lifetime T2{T}_{2}T2​ in powders.
We observe the two- and three-pulse photon echo emission from a scattering powder, obtained by grinding a Pr3+:Y2SiO5 rare earth doped single crystal. We show that the collective emission is coherently constructed over several grains. A well defined atomic coherence can therefore be created between randomly placed particles. Observation of photon echo on powders as opposed to bulk materials opens the way to faster material development. More generally, time-domain resonant four-wave mixing offers an attractive approach to investigate coherent propagation in scattering media.
A theoretical model for superradiant damping effect in inhomogeneously broadened media and its application to photon-echo problems are discussed. Only optically thin systems are considered, and all nonradiative relaxation mechanisms are neglected. Numerical calculations are performed for a very wide square inhomogeneous line shape and square applied pulses. It is shown that excitation of the system becomes increasingly difficult as the superradiant lifetime ${\ensuremath{\tau}}_{s}$ becomes comparable with T2∗{T}_{2}^{*}T2∗​. The energy reradiated after the end of the exciting pulse is considerable for ${\ensuremath{\tau}}_{s}\ensuremath{\approx}{T}_{2}^{*}$ and for some applied pulse areas. Two-pulse sequences produce multiple echoes as the microscopic polarizations spontaneously rephase. The first-echo amplitude maximum is found to occur for first-applied-pulse areas increasingly above $\frac{1}{2}\ensuremath{\pi}$ as ${\ensuremath{\tau}}_{s}$ decreases. For a given first-pulse area, the echo intensities increase initially as ${\ensuremath{\tau}}_{s}$ decreases (negligible damping) and finally decrease and vanish (important damping). The ratio of the second- to first-echo amplitudes is found to be proportional to $\frac{{T}_{2}^{*}}{{\ensuremath{\tau}}_{s}}$ for small superradiance levels and to decrease when ${\ensuremath{\tau}}_{s}$ approaches T2∗{T}_{2}^{*}T2∗​. An approximate estimate of this ratio is derived for the region of linearity in $\frac{{T}_{2}^{*}}{{\ensuremath{\tau}}_{s}}$.
The active use of resonators in quantum technologies increases the interest of their application in the creation of optical and microwave quantum memory. The use of photon and spin echoes opens up the possibility of storing a large number of light pulses in one such memory cell. High efficiency of such quantum memory is achieved in an optically dense resonant media, in which the formation of a photon (spin) echo can be accompanied by an increase in the nonlinear interaction of light with atoms causing the appearance of multiple echo signals. In this paper, we develop the pulse area approach to study general nonlinear properties of the primary and multi-pulse echo signals excited in a two-level atomic ensemble located in ring cavities with volumetric and surface modes. Conditions under which one or more echo pulses can be generated are analyzed. The solutions obtained are compared with recent experimental results. We show that the area theorem is one of the simplest and most powerful analytical tools for studying a highly nonlinear and dynamical process of the formation of the sequence of photon/spin echo signals in resonant media inside the resonator.
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.
The authors derive analytical expressions for secondary echoes formed under the two-pulse excitation of the optically dense media developing McCall-Hahn area theorem for echo effects. They find that a series of self-reviving echo signals with a total area of 2$\ensuremath{\pi}$ or 0$\ensuremath{\pi}$ is excited and propagates deep in the media demonstrating strong non-linear nature of light-matter interaction at small changes of second pulse area. The pulse area approach paves the way for precise coherent spectroscopy, the study of different photon echoes and quantum control of light pulses in the optically dense media.