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Yonatan Sivan

Publications and source records attributed to Yonatan Sivan.

At least 37 records · Page 2Linked to original sources
arXiv2020

An efficient solver for the generalized normal modes of non-uniform open optical resonators

Modal expansion is an attractive technique for solving electromagnetic scattering problems. With the one set of resonator modes, calculated once and for all, any configuration of near-field or far-field sources can be obtained almost instantaneously. Traditionally applied to closed systems, a simple and rigorous generalization of modal expansion to open systems using eigenpermittivity states is also available. These open modes are suitable for typical nanophotonic systems, for example. However, the numerical generation of modes is usually the most difficult and time-consuming step of modal expansion techniques. Here, we demonstrate efficient and reliable mode generation, expanding the target modes into the modes of a simpler open system that are known. Such a re-expansion technique is implemented for resonators with non-uniform permittivity profiles, demonstrating its rapid convergence. Key to the method's success is the inclusion of a set of longitudinal basis modes.

physics.optics↗
arXiv2019

Overcoming the bottleneck for quantum computations of complex nanophotonic structures: Purcell and FRET calculations using a rigorous mode hybridization method

A calculation of the photonic Green's tensor of a structure is at the heart of many photonic problems, but for non-trivial nanostructures, it is typically a prohibitively time-consuming task. Recently, a general normal mode expansion (GENOME) was implemented to construct the Green's tensor from eigenpermittivity modes. Here, we employ GENOME to the study the response of a cluster of nanoparticles. To this end, we use the rigorous mode hybridization theory derived earlier by D. J. Bergman [Phys. Rev. B 19, 2359 (1979)], which constructs the Green's tensor of a cluster of nanoparticles from the sole knowledge of the modes of the isolated constituent. The method is applied, for the first time, to a scatterer with a non-trivial shape (namely, a pair of elliptical wires) within a fully electrodynamic setting, and for the computation of the Purcell enhancement and Förster Resonant Energy Transfer (FRET) rate enhancement, showing a good agreement with direct simulations. The procedure is general, trivial to implement using standard electromagnetic software, and holds for arbitrary shapes and number of scatterers forming the cluster. Moreover, it is orders of magnitude faster than conventional direct simulations for applications requiring the spatial variation of the Green's tensor, promising a wide use in quantum technologies, free-electron light sources and heat transfer, among others.

physics.comp-ph↗
arXiv2019

Second-harmonic generation due to coulomb-like interaction in a heterodimer of subwavelength dimensions

We experimentally study the optical second harmonic generation (SHG) from deep subwavelength gold-silver heterodimer and silver-silver and gold-gold homodimers. Our results show that the SHG from the heterodimer is about an order of magnitude more intense. In contrast, calculations based on known theory suggest that it is the silver-silver homodimer that should have the upper hand, putting the present theoretical view at odds with our experimental findings. Following this observation, we propose a dynamic model where nonlinearity emerges not from the material particles themselves but form the Coulombic interaction between them that prevailed over other nonlinear optics mechanisms at the extreme subwavelength dimensions of the dimer in this case. The model's good agreement, combined with the failure of the conventional theoretical view, implies a yet uncharted nonlinear optical effect.

physics.optics↗
arXiv2019

"Hot" electrons in metallic nanostructures -- non-thermal carriers or heating?

Understanding the interplay between illumination and the electron distribution in metallic nanostructures is a crucial step towards developing applications such as plasmonic photo-catalysis for green fuels, nano-scale photo-detection and more. Elucidating this interplay is challenging, as it requires taking into account all channels of energy flow in the electronic system. Here, we develop such a theory, which is based on a coupled Boltzmann-heat equations and requires only energy conservation and basic thermodynamics, where the electron distribution, and the electron and phonon (lattice) temperatures are determined {\em uniquely}. Applying this theory to realistic illuminated nanoparticle systems, we find that the electron and phonon temperatures are similar, thus justifying the (classical) single temperature models. We show that while the fraction of high-energy ``hot'' carriers compared to thermalized carriers grows substantially with illumination intensity, it remains extremely small (on the order of $10^{-8}$). Importantly, most of the absorbed illumination power goes into heating rather than generating hot carriers, thus rendering plasmonic hot carrier generation extremely inefficient. Our formulation allows for the first time a unique quantitative comparison of theory and measurements of steady-state electron distributions in metallic nanostructures.

physics.optics↗
arXiv2019

Eppur si riscalda -- and yet, it (just) heats up: Further Comments on "Quantifying hot carrier and thermal contributions in plasmonic photocatalysis"

Our Comment [Sivan et al., Science 2019] (as well as its longer version [Dubi, Un, & Sivan, ArXiv 2019], and the supporting theoretical studies [Dubi and Sivan, ArXiv 2018]) on recent attempts to distinguish thermal and non-thermal ("hot carrier") contributions to plasmon-assisted photocatalysis [Zhou et al., Science 2018] initiated a re-evaluation process of previous literature on the topic within the nano-plasmonics and chemistry communities. The Response of Zhou et al. attempts to defend the claims of the original paper. In this manuscript, we show that the Response presents additional data that further validates our central criticism: inaccurately measured temperatures (that are lower than the actual temperature of the catalyst) led Zhou et al. to incorrectly claim conclusive evidence of non-thermal effects. We identify flaws in the experimental setup (e.g. the use of the default settings for the thermal camera and incorrect positioning of the thermometer) that may have led Zhou et al. to make such claims. We further show that the Response contains several factual errors and does not address the technical problems we identified with the data acquisition in [Zhou et al., Science 2018]. We demonstrate that both the Response and the original paper contain additional faults, for example, in the power determination and in the normalization of the rate to the catalyst volume, and exhibit misconceptions regarding the thermo-optic response of metal nanostructures. The burden of proof required by the proposal of a novel physical mechanism has simply not been met, especially when the existing data can be modeled exquisitely by conventional theory.

physics.chem-ph↗
arXiv2019

Size-Dependence of the photothermal response of a single metal nanosphere

We study the thermal response of a single spherical metal nanoparticle to continuous wave illumination as a function of its size. We show that the particle temperature increases non-monotonically as the particle size increases, indicating that the photo-thermal response can be optimized by tuning the particle size and illumination wavelength. We also compare the size-effect on the photo-thermal effects of gold and silver nanoparticles and find somewhat surprisingly that Ag NPs are more efficient heat generators only for sufficiently small sizes. These results have importance primarily for application such as plasmon-assisted photo-catalysis, photothermal cancer therapy, etc., and provide a first step toward the study of the size-dependence of the thermo-optic nonlinearity of metal nanospheres.

physics.optics↗
arXiv2019

Thermal effects - an alternative mechanism for plasmonic-assisted photo-catalysis

Recent experiments claimed that the enhancement of catalytic reaction rates occurs via the reduction of activation barriers driven by non-equilibrium (``hot'') electrons in plasmonic metal nanoparticles. These experiments place plasmonic photo-catalysis as a promising path for enhancing the efficiency of various chemical reactions. Here, we argue that what appears to be photo-catalysis is in fact thermo-catalysis, driven by the well-known plasmon-enhanced ability of illuminated metallic nanoparticles to serve as heat sources. Specifically, we point to some of the most important papers in the field, and show that a simple theory of illumination-induced heating can explain the extracted experimental data to remarkable agreement, with minimal to no fit parameters. We further show that any small temperature difference between the photocatalysis experiment and a control experiment performed under uniform external heating is effectively amplified by the exponential sensitivity of the reaction, and very likely to be interpreted incorrectly as ``hot'' electron effects.

physics.chem-ph↗
arXiv2019

Surface second-harmonic from metallic nanoparticle configurations - a transformation optics approach

We study surface second-harmonic generation (SHG) from a singular plasmonic structure consisting of touching metallic wires. We use the technique of transformation optics and relate the structure to a rather simpler geometry, a slab waveguide. This allows us to obtain an analytical solution to the problem, revealing rich physical insights. We identify various conditions that govern the SHG efficiency. Importantly, our analysis demonstrates that apart from the mode-matching condition, phase-matching condition is relevant even for this sub-wavelength structure. Furthermore, we identify a geometric factor which was not identified before. We support our analysis with numerical simulations.

physics.optics↗
arXiv2018

Tracking ultrafast hot-electron diffusion in space and time by ultrafast thermo-modulation microscopy

The ultrafast response of metals to light is governed by intriguing non-equilibrium dynamics involving the interplay of excited electrons and phonons. The coupling between them gives rise to nonlinear diffusion behavior on ultrashort timescales. Here, we use scanning ultrafast thermo-modulation microscopy to image the spatio-temporal hot-electron diffusion in a thin gold film. By tracking local transient reflectivity with 20 nm and 0.25 ps resolution, we reveal two distinct diffusion regimes, consisting of an initial rapid diffusion during the first few picoseconds after optical excitation, followed by about 100-fold slower diffusion at longer times. We simulate the thermo-optical response of the gold film with a comprehensive three-dimensional model, and identify the two regimes as hot-electron and phonon-limited thermal diffusion, respectively.

physics.optics↗
arXiv2017

Generalizing normal mode expansion of electromagnetic Green's tensor to lossy resonators in open systems

We generalize normal mode expansion of Green's tensor $\bar{\bar{G}}(\bf{r},\bf{r}')$ to lossy resonators in open systems, resolving a longstanding open challenge. We obtain a simple yet robust formulation, whereby radiation of energy to infinity is captured by a complete, discrete set of modes, rather than a continuum. This enables rapid simulations by providing the spatial variation of $\bar{\bar{G}}(\bf{r},\bf{r}')$ over both $\bf{r}$ and $\bf{r}'$ in one simulation. Few eigenmodes are often necessary for nanostructures, facilitating both analytic calculations and unified insight into computationally intensive phenomena such as Purcell enhancement, radiative heat transfer, van der Waals forces, and Förster resonance energy transfer. We bypass all implementation and completeness issues associated with the alternative quasinormal eigenmode methods, by defining modes with permittivity rather than frequency as the eigenvalue. We obtain true stationary modes that decay rather than diverge at infinity, and are trivially normalized. Completeness is achieved both for sources located within the inclusion and the background through use of the Lippmann-Schwinger equation. Modes are defined by a linear eigenvalue problem, readily implemented using any numerical method. We demonstrate its simple implementation on COMSOL Multiphysics, using the default inbuilt tools. Results were validated against direct scattering simulations, including analytical Mie theory, attaining arbitrarily accurate agreement regardless of source location or detuning from resonance.

physics.optics↗
arXiv2017

Revisiting the boundary conditions for second-harmonic generation at metal-dielectric interfaces

We study second-harmonic generation (SHG) arising from surface nonlinearity at a metal-dielectric interface using a spectral decomposition method. Since our method avoids the need to consider the generalized boundary condition across the metal-dielectric interface in the presence of a perpendicular surface source, we retrieve the known discontinuity of the tangential component of the electric field ($E_{\parallel}^ {2ω}$) for a general geometry, based on a purely mathematical argument. Further, we reaffirm the standard convention of the implementation of this condition, namely, that the surface dipole source radiates as if placed outside the metal surface for arbitrary geometries. We also study and explain the spectral dependence of the discontinuity of the tangential component of the electric field at second harmonic. Finally, we note that the default settings of the commercial numerical package COMSOL Multiphysics fail to account for the $E_{\parallel}^ {2ω}$-discontinuity. We provide a simple recipe that corrects the boundary condition within these existing settings.

physics.optics↗
arXiv2016

Nanoparticle-assisted STED nanoscopy with gold nanospheres

We demonstrate stimulated emission depletion (STED) microscopy with 20 nm gold nanospheres coated by fluorescent silica. Compared with previous demonstrations of STED with a hybrid plasmonic fluorescent label, the current implementation offers a substantially smaller label and a better resolution improvement of up to 2.5-fold beyond the diffraction limit of confocal microscopy. This is achieved at approximately 2 times lower intensity than conventional STED based on dyes alone, and in an aqueous environment, demonstrating the relevance to bio-imaging. Finally, we also show, for the first time in this context, a 3-fold reduction in the rate of photobleaching compared to standard dye-based STED, thus, enabling brighter images.

physics.optics↗
arXiv2016

Plasmonic nanoprobes for stimulated emission depletion microscopy

Plasmonic nanoparticles influence the absorption and emission processes of nearby emitters due to local enhancements of the illuminating radiation and the photonic density of states. Here, we use the plasmon resonance of metal nanoparticles in order to enhance the stimulated depletion of excited molecules for super-resolved microscopy. We demonstrate stimulated emission depletion (STED) microscopy with gold nanorods with a long axis of only 26 nm and a width of 8 nm that provide an enhancement of the resolution compared to fluorescent-only probes without plasmonic components irradiated with the same depletion power. These novel nanoparticle-assisted STED probes represent a ~2x10^3 reduction in probe volume compared to previously used nanoparticles and we demonstrate their application to the first plasmon-assisted STED cellular imaging. We also discuss their current limitations.

physics.optics↗
arXiv2016

Temperature-dependent permittivity of annealed and unannealed gold films

Due to local field enhancement and subwavelength confinements, nano-plasmonics provide numerous novel applications. Simultaneously, as an efficient nanoscale heat generator from inherent absorption, thermo-plasmonics is emerging as an important branch. However, although significant temperature increase is involved in applications, detailed characterization of metal permittivity at different temperatures and corresponding thermo-derivative are lacking. In this work, we extract the permittivity of gold from 300K to the annealing temperature of 570K. By comparing annealed and unannealed films, more than one-order difference in thermo-derivative of permittivity is revealed, resulting in unexpectedly large variation of plasmonic properties. Our result is valuable not only for characterizing extensively used unannealed nanoparticles, but also for designing future thermo-nano-plasmonic systems.

physics.optics↗
arXiv2016

Robust Location of Optical Fiber Modes via the Argument Principle Method

We implement a robust, globally convergent root search method for transcendental equations guaranteed to locate all complex roots within a specified search domain, based on Cauchy's residue theorem. Although several implementations of the argument principle already exist, ours has several advantages: it allows singularities within the search domain and branch points are not fatal to the method. Furthermore, our implementation is simple and is written in MATLAB, fulfilling the need for an easily integrated implementation which can be readily modified to accommodate the many variations of the argument principle method, each of which is suited to a different application. We apply the method to the step index fiber dispersion relation, which has become topical due to the recent proliferation of high index contrast fibers. We also find modes with permittivity as the eigenvalue, catering to recent numerical methods that expand the radiation of sources by eigenmodes.

physics.comp-ph↗
arXiv2016

Nonlinear plasmonics at high temperatures

We solve the Maxwell and heat equations self-consistently for metal nanoparticles under intense continuous wave (CW) illumination. Unlike previous studies, we rely on {\em experimentally}-measured data for the metal permittivity for increasing temperature and for the visible spectral range. We show that the thermal nonlinearity of the metal can lead to substantial deviations from the predictions of the linear model for the temperature and field distribution, and thus, can explain qualitatively the strong nonlinear scattering from such configurations observed experimentally. We also show that the incompleteness of existing data of the temperature dependence of the thermal properties of the system prevents reaching a quantitative agreement between the measured and calculated scattering data. This modelling approach is essential for the identification of the underlying physical mechanism responsible for the thermo-optical nonlinearity of the metal and should be adopted in all applications of high temperature nonlinear plasmonics, especially for refractory metals, both for CW and pulsed illumination.

physics.optics↗
arXiv2016

Reinterpreting the magnetoelectric coupling of polarizability tensors of infinite cylinders using symmetry: a simple TM/TE view

Recently, Strickland et al retrieved dynamic polarizabilities of infinitely long wires at oblique incidence, reporting non-zero magnetoelectric coupling, seemingly defying existing theorems which forbid this in centrosymmetric scatterers. We reconcile this finding with existing symmetry restrictions on microscopic polarizabilities using a property of line dipoles. This motivates a reformulation of cylinder polarizability, yielding diagonal tensors that decompose the response into TM and TE contributions, simplifying subsequent treatment by homogenization theories. A transformation is derived between Strickland et al.'s formulation and our reformulation, allowing magnetoelectric coupling to be identified as the contrast between TM and TE responses, and enabling simple geometric insights into all its scaling and symmetry properties.

physics.optics↗