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Conference on Lasers and Electro-Optics

Delayed luminescence from mesoscopic scattering media

Mahed Batarseh, Zhean Shen, Aristide C. Dogariu

Published Jan 1, 2022• 0 citations
Publisher

Abstract

We demonstrate experimentally and numerically that many-body interactions between nanosized colloidal particles lead to subradiant regimes where the lifetime of emission long after the excitation ceases depends on the average particle-particle distance.
DOI
10.1364/cleo_qels.2022.fth4d.5

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The objective of this thesis is to expand our understanding of collective light-scattering phenomena, which manifest themselves in the strong suppression of radiation from the scattering medium. In particular, we are interested in subradiance, a collective effect in spontaneous emission which, as a result of the dissipative coupling of atoms through common electromagnetic modes, creates long-lived excitation modes in an ensemble of cold atoms, with lifetimes much longer than those of individual, isolated atoms. Previously, subradiance had been well-characterized for dilute cold-atom scattering media and the low-intensity limit of the driving laser (linear-optics regime). In this thesis, we study this collective phenomenon beyond the linear-optics and dilute regimes.To study experimentally subradiance beyond the linear-optics regime, we varied the saturation parameter of the excitation laser up to relatively large values and we have observed the increase of the subradiant population with increasing saturation parameter. More importantly, we have identified the super-linear scaling of the subradiant population beyond the linear-optics regime, due to a process similar to optical pumping via multi-excitation superradiant states. This study showed that the increase in the intensity of the driving laser beyond the linear-optics regime can overcome the weak coupling of subradiant modes with the external world.Moreover, we have numerically studied subradiance using the vectorial coupled-dipole model, with a focus on understanding the effect of the near-field dipole-dipole interaction. For that, we extensively compared the vectorial and scalar (which does not contain near-field interaction terms) models and studied the subradiant lifetime as a function of the density and optical thickness of the cold-atom cloud. We observed that the near-field terms are detrimental for subradiance, which was seen in the reduction of the subradiant lifetimes with increasing density. This detrimental character of near-field terms can be interpreted as being due to an effective inhomogeneous broadening induced by the near-field interaction, which reduces the subradiant lifetimes as the density increases.The detrimental character of near-field interaction has also been previously numerically identified for Anderson localization of light waves (Anderson localization is a coherent multiple-scattering wave phenomenon in a strongly scattering medium that results in a cessation of a diffusive wave transport; it also yields long-lived modes): the scalar coupled-dipole model predicts Anderson localization of light waves, but not the vectorial one. However, adding a strong magnetic field allows one to recover localized modes for vectorial light. In this context, we numerically studied a possible signature of Anderson localization of light in cold atoms, based on the measurement of intensity fluctuations of the scattered light. We have shown that at the transition to the localized regime, the fluctuations are enhanced. In particular, for vectorial light, we have demonstrated the absence and recovery of enhanced intensity fluctuations without and with the applied magnetic field, which further corroborates that the intensity fluctuations could serve as an experimental way to probe the localized states.
Spontaneous emission rate is not only affected by the properties of the material itself, but also depends on the dielectric properties of the surrounding media. Recently, some work has been carried out to study the dependence of spontaneous emission rates of the luminescent-ion-containing nanometer particles on the refractive index of the media. Based on the free distribution of nanometer particles in media, the pro-bability density of luminescent lifetime is analyzed. Since nanometer particles distribute freely in media, the number of nanometer particles in a given volume surrounding the luminescent center obeys the Poission distribution. The local relative refractive index nr, which is the ratio of media effective refractive index to particle refractive index, is affected by the particle number of nanoparticles within a sphere of radius half of the radiative wavelength. The probability density function of nr can be obtained according to the dependence of nr on the particle number. Based on the relation between nr and luminescence lifetime, the analytical form of probability density function of lifetime is obtained. A calculation has been done based on the parameters given in Meltzer's experiment (Eu3+ doped Y2O3 in methanol). The result shows that the relative fluctuation of luminescence lifetime is too small to be observed. However, with increasing size of nanometer particles or density of nanometer particles, the relative fluctuation of lifetime increases greatly and could be observed.
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.