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Journal of the Optical Society of America B

Electrical generation of stationary light in random scattering media

Shawn M. Redmond, G. L. Armstrong, H.-Y. Chan, Emily Minton Mattson, A. Mock, B. Li, J. R. Potts, Meng Cui, Stephen Colby Rand, Samuel L. Oliveira, Julien Marchal, T. Hinklin, Richard M. Laine

Published Jan 1, 2004• 15 citations
Publisher

Abstract

In recent years there has been great interest in controlling the speed of propagation of electromagnetic waves. In gases and crystals, coherent techniques have been applied to alter the speed of light without changing the physical or chemical structure of the medium. Also, light transmitted by highly disordered solids has exhibited signatures of Anderson localization, indicating the existence of a regime of “stopped” light that is mediated by random elastic scattering. However, to date, light has not been generated in a random medium as a pointlike excitation that is fixed in space from the outset. Here we report experimental evidence for the electrical generation and confinement of light within nanosized volumes of a random dielectric scattering medium in which a population inversion has been established, and discuss the properties of these novel light sources.

DOI
10.1364/josab.21.000214

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In recent years there has been great interest in controlling the speed of propagation of electromagnetic waves. In gases and crystals, coherent techniques have been applied to alter the speed of light without changing the physical or chemical structure of the medium. Also, light transmitted by highly disordered solids has exhibited signatures of Anderson localization, indicating the existence of a regime of “stopped” light that is mediated by random elastic scattering. However, to date, light has not been generated in a random medium as a pointlike excitation that is fixed in space from the outset. Here we report experimental evidence for the electrical generation and confinement of light within nanosized volumes of a random dielectric scattering medium in which a population inversion has been established, and discuss the properties of these novel light sources.
Light propagation in matter is described by vibration eigenstates, called modes, which characterize the light-matter interaction. In the specific case of random media, according to the strength of the disorder, the modes can be either extended over the whole system or spatially localized. This disorder-based confinement is called Anderson’s localization.In the first part, we introduce basic notions used along this manuscript. In particular the light-matter interaction requires a semiclassical approach: The electromagnetic field is described by Maxwell’s equations while the quantum nature of matter must be considered. In this thesis open media are studied. In such systems the modal description requires a specific analytic treatment different from closed problems. In the second part, we focus on Anderson-localized modes in open passive random media. Any change of the disorder induces modifications of modes. Therefore, it enables the control over the light properties. Moreover, when inserting an emitter inside an Anderson-localized mode, strong light-matter interaction regimes can be reached. In the third part, active random media, commonly called random lasers, are introduced. Using our experimental achievements, characteristics of random lasers are presented. The notion of mode enables us to describe complex mechanisms involved in the lasing emission. Last, we demonstrate both experimentally and numerically that a non-uniform excitation of random lasers can lead to a control of the properties of the emission. In particular a multimode spectrum for a uniform pumping can be turned into single-mode using an adapted pumping.
In the last decade Anderson Localization of Light and Random Lasing has attracted a variety of interest in the community of condensed matter theory. The fact that a system so inartificial as a thin layer consisting of dust particles, which have amplifying properties, can produce coherent laser emission, is of a simple elegance, which promises new insights in fundamental physics. There is no need of an external feedback mechanism, like in the system of a conventional laser. Whereas several attempts try to enter the subject numerically by considering cavity approximations, this thesis is concerned with building a microscopically self-consistent theory of random lasing. Designing this method, we had to study light localization effects in random media including absorption and gain. Incorporating interference effects by means of Cooperon contributions we derived Anderson localized states for passive media. Mapping this on a system which consists of laser active Mie-scatterers in a passive medium, we found that by incorporation of the Cooperon, we loose the Anderson localization, but the system is weakly localized, which is sufficient for population inversion and stimulated emission.
We investigated several types of random lasing modes against frequency and the excitation of active medium. Random lasing occurring from multiple light scatterings and the interference effect of the scattered light has various complex lasing states in disordered structures, in which light waves are localized in various forms. Modes of random lasing are generally classified into localized, extended and transition modes based on their localization types. Numerical methods are used for analysing such complex phenomena. In this paper, a finite-element method is used to investigate the relationship among lasing modes, frequency and population inversion density of active medium for random lasing. Light amplification defined as the ratio of radiative powers between excited and non-excited states of the active medium is computed by changing both the frequency and the population inversion density of the active medium, which is modelled by the negative imaginary part of relative permittivity. The distributions of random lasing modes is strongly influenced by the lasing frequency. We also found that the localized modes that are strongly confined lasing modes in disordered structures do not appear in the frequency ranges in which mean free paths are approximately equal to the half-wavelength.
Summary form only given. Over the past two decades, there has been much progress in the study of light transport in a disordered dielectric medium. Most studies are within the framework of ray optics or wave optics. Quantum statistical properties of light in a random medium have received little attention. To bridge the gap between random media and quantum optics, we conducted an experimental study of photon statistics of random lasers. ZnO nanoparticles with an average diameter of 80 nm are cold-pressed to form a pellet. In the coherent backscattering experiment, the scattering mean free path is measured The frequency-tripled output of a picosecond Nd:YAG laser is used to optically excite the ZnO pellet. The ZnO emission is measured by a spectrometer which is connected to a streak camera.
The study of optical effects in active media is rich with unexpected consequences. For instance, one may imagine that absorption and amplification in a dielectric medium will exhibit some sort of symmetry because both are related to the same imaginary part of the dielectric constant, except for a sign change. It turns out that such a symmetry does not exist [1]. This issue has also been investigated in detail for random or disordered gain media, with varying viewpoints [2]. Traditionally, much of the research on amplifying media has considered the interaction of light within the entire volume of such a medium. Recent interest in metamaterials and other esoteric structures in which plasmons are used to manipulate optical signals has brought attention to the role of surface waves in active dielectrics [3, 4]. From a fundamental perspective, the main difference between active and passive media is that spontaneous emission cannot be avoided in gain media. As a result, a rigorous analysis of gain media demands a quantum-mechanical treatment. Spontaneous emission in a gain medium depends not only on the material properties of that medium but also on the optical modes supported by the structure containing that material [5]. By a clever design of this structure (e.g., photonic crystals or microdisk resonators with a metallic cladding), it is possible to control the local density of optical modes and the spontaneous emission process itself. In Chapter 4, we discuss how to model a gain medium under such conditions by deploying optical Bloch equations.
We report on a medium exhibiting extremely efficient light scattering properties: a liquid network formed in a porous matrix. Liquid fragments confined in the solid matrix result in a random fluctuation of the dielectric function and act as scattering objects for photons. The optical scattering efficiency is defined by the filling factor of the liquid in the pores and its dielectric constant. The spectral dependence of the scattering length of photons indicates that the phenomenon is governed by a Mie-type scattering mechanism. The degree of the dielectric disorder of the medium, i.e. the level of opacity is tunable by the ambient vapor pressure of the dielectric substance. In the strongest scattering regime the scattering length of photons is found to be in the micrometer range. By incorporation of dye molecules in the voids of the porous layer a system exhibiting optical gain is realized. In the multiple scattering regime the optical path of diffusively propagating photons is enhanced and light amplification through stimulated emission occurs: a strong intensity enhancement of the dye emission accompanied by significant spectral narrowing is observed above the excitation threshold for a layer being in the opalescence state. (© 2005 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim)