Large Fluorescence Enhancement via Lossless All-Dielectric Spherical Mesocavities.

Nano- and microparticles are popular media to enhance optical signals, including fluorescence from a dye proximal to the particle. Here we show that homogeneous, lossless, all-dielectric spheres with diameters in the mesoscale range, between nano- (≲100 nm) and micro- (≳1 µm) scales, can offer surprisingly large fluorescence enhancements, up to F ∼ 104. With the absence of nonradiative Ohmic losses inherent to plasmonic particles, we show that F can increase, decrease or even stay the same with increasing intrinsic quantum yield q0, for suppressed, enhanced or intact radiative decay rates of a fluorophore, respectively. Further, the fluorophore may be located inside or outside the particle, providing additional flexibility and opportunities to design fit for purpose particles. The presented analysis with simple dielectric spheres should spur further interest in this less-explored scale of particles and experimental investigations to realize their potential for applications in imaging, molecular sensing, light coupling, and quantum information processing.

Extraordinary Fluorescence Enhancement in Metal-Dielectric Core-Shell Nanoparticles.

We show that in metal-dielectric core-shell nanoparticles, unusually thick dielectric coatings can produce extreme fluorescence enhancement with an enhancement factor F̅ ≳ 3000 for emitters located on the surface or in the interior of the shell of Au@dielectric spherical particles under realistic conditions, even for the emitters with 100% intrinsic quantum yield. Thick dielectric coatings facilitate high-quality transverse electric (TE) multipole (l = 7) resonances which are shown as the major cause for the reported extraordinary values of F̅.

Intriguing branching of the maximum position of the absorption cross section in Mie theory explained.

A potential control over the position of maxima of scattering and absorption cross sections can be exploited to better tailor nanoparticles for specific light-matter interaction applications. Here we explain in detail the mechanism of an appreciable blue shift of the absorption cross-section peak relative to a metal spherical particle localized surface plasmon resonance (LSPR) defined as the maximum of the extinction (and scattering) cross section. Such a branching of cross sections' maxima requires a certain threshold value of size parameter (x≈0.7 for dipole channel) and is a prerequisite for obtaining high fluorescence enhancements, because the spectral region of high radiative rate enhancement becomes separated from the spectral region of high non-radiative rate enhancement. A consequence is that the maximum of the absorption cross section cannot be used as the definition of the LSPR position for x≳0.7.

Electromagnetic energy in multilayered spherical particles.

We obtain exact analytic expressions for (i) the electromagnetic energy radial density within and outside a multilayered sphere and (ii) the total electromagnetic energy stored within its core and each of its shells. Explicit expressions for the special cases of lossless core and shell are also provided. The general solution is based on the compact recursive transfer-matrix method, and its validity includes also magnetic media. The theory is illustrated on examples of electric field enhancement within various metallo-dielectric silica-gold multilayered spheres. The user-friendly MATLAB code, which includes the theoretical treatment, is available as a supplement to the paper.

Distance dependence of single-fluorophore quenching by gold nanoparticles studied on DNA origami.

We study the distance-dependent quenching of fluorescence due to a metallic nanoparticle in proximity of a fluorophore. In our single-molecule measurements, we achieve excellent control over structure and stoichiometry by using self-assembled DNA structures (DNA origami) as a breadboard where both the fluorophore and the 10 nm metallic nanoparticle are positioned with nanometer precision. The single-molecule spectroscopy method employed here reports on the co-localization of particle and dye, while fluorescence lifetime imaging is used to directly obtain the correlation of intensity and fluorescence lifetime for varying particle to dye distances. Our data can be well explained by exact calculations that include dipole-dipole orientation and distances. Fitting with a more practical model for nanosurface energy transfer yields 10.4 nm as the characteristic distance of 50% energy transfer. The use of DNA nanotechnology together with minimal sample usage by attaching the particles to the DNA origami directly on the microscope coverslip paves the way for more complex experiments exploiting dye-nanoparticle interactions.

High trapping forces for high-refractive index particles trapped in dynamic arrays of counterpropagating optical tweezers.

We demonstrate the simultaneous trapping of multiple high-refractive index (n > 2) particles in a dynamic array of counterpropagating optical tweezers in which the destabilizing scattering forces are canceled. These particles cannot be trapped in single-beam optical tweezers. The combined use of two opposing high-numerical aperture objectives and micrometer-sized high-index titania particles yields an at least threefold increase in both axial and radial trap stiffness compared to silica particles under the same conditions. The stiffness in the radial direction is obtained from measured power spectra; calculations are given for both the radial and the axial force components, taking spherical aberrations into account. A pair of acousto-optic deflectors allows for fast, computer-controlled manipulation of the individual trapping positions in a plane, while the method used to create the patterns ensures the possibility of arbitrarily chosen configurations. The manipulation of high-index particles finds its application in, e.g., creating defects in colloidal photonic crystals and in exerting high forces with low laser power in, for example, biophysical experiments.

Improvement of Mishchenko's T-matrix code for absorbing particles.

The use of Gaussian elimination with backsubstitution for matrix inversion in scattering theories is discussed. Within the framework of the T-matrix method (the state-of-the-art code by Mishchenko is freely available at http://www.giss.nasa.gov/-crmim), it is shown that the domain of applicability of Mishchenko's FORTRAN 77 (F77) code can be substantially expanded in the direction of strongly absorbing particles where the current code fails to converge. Such an extension is especially important if the code is to be used in nanoplasmonic or nanophotonic applications involving metallic particles. At the same time, convergence can also be achieved for large nonabsorbing particles, in which case the non-Numerical Algorithms Group option of Mishchenko's code diverges. Computer F77 implementation of Mishchenko's code supplemented with Gaussian elimination with backsubstitution is freely available at http://www.wave-scattering.com.

Negative refractive index metamaterials from inherently non-magnetic materials for deep infrared to terahertz frequency ranges.

We present a new set of artificial structures which can exhibit a negative refractive index band in excess of 6% in a broad frequency range from the deep infrared to the terahertz region. The structures are composites of two different kinds of non-overlapping spheres, one made from inherently non-magnetic polaritonic and the other from a Drude-like material. The polaritonic spheres are responsible for the existence of negative effective magnetic permeability whilst the Drude-like spheres are responsible for negative effective electric permittivity. The resulting negative refractive index structures are truly subwavelength structures with wavelength-to-structure ratio 14:1, which is almost 50% higher than has been previously achieved. Our results are explained in the context of the extended Maxwell-Garnett theory and are reproduced by calculations based on the layer Korringa-Kohn-Rostoker method, an ab initio multiple scattering theory. The role of absorption in the constituent materials is discussed. Effective medium computer F77 code is freely available at http://www.wave-scattering.com.

Aspect Ratio Analysis for Ground States of Bosons in Anisotropic Traps.

Characteristics of the initial condensate in the recent experiment on Bose-Einstein condensation (BEC) of 87Rb atoms in an anisotropic magnetic trap are discussed. Given the aspect ratio R, the quality of BEC is estimated. A simple analytical ansatz for the initial condensate wave function is proposed as a function of the aspect ratio which, in contrast to the Baym-Pethick trial wave function, can be used for any interaction strength, reproduces both the weak and the strong interaction limits, and which is in better agreement with numerical results than the latter.