Searcharxiv⌕ Search

arXiv subjects

Zoltan Sztranyovszky

Publications and source records attributed to Zoltan Sztranyovszky.

6 recordsLinked to original sources

Accessing both electrochemical SEIRA and SERS with ultrasensitive metamaterials for enhanced molecular identification

Surface-enhanced IR absorption (SEIRA) and surface-enhanced Raman spectroscopy (SERS) are complementary techniques that allow for ultrasensitive chemical fingerprinting. Non-invasive optical sensing would be significantly improved by a robust implementation of a reusable substrate that combines these techniques. Here, we present an electrochemically-cleanable metamaterial that enables combined real-time SEIRA and SERS in flow. This metamaterial facilitates the study of surface-adsorbed species and diffusion layers, elicits spectral shifts from changes in nanogap refractive index of 1400 nm/RIU, and delivers ultrasensitive analyte detection. Combining SERS and SEIRA clarifies molecular (electro)chemical transformations and tracks changes in selection rules and symmetry breaking at the analyte-electrode interface. This development in enhanced multimodal spectro-electrochemistry is suited for multiple domains, including understanding charge transport mechanisms and interfacial dynamics at electrodes, and is capable of real-time flow monitoring for a wide range of molecular processes.

physics.optics↗

Extreme mid-infrared field enhancement and anapoles in high-index plasmonic metamaterials

High-refractive-index materials underpin a wide range of optical technologies, including communications, imaging, lasers, and integrated photonic systems. Here, we demonstrate a self-assembled metamaterial platform based on gold nanoparticle aggregates with nanometer-scale gaps exhibit remarkably high effective refractive indices exceeding 15 in the mid-infrared regime, while simultaneously producing gap-field enhancements of at least two-orders of magnitude. This combination of high refractive index and extreme field enhancement enables exceptionally strong light-matter interactions. We demonstrate this by designing a compact high-index metamaterial device supporting an anapole, which further enhances the nanogap field. By placing quantum emitters with terahertz transitions inside the plasmonic gaps, we show a stimulated-emission response enhanced by at least three orders of magnitude, highlighting applications in non-linear optics, frequency up-conversion and vibrational strong coupling.

physics.optics↗

Extending completeness of the eigenmodes of an open system beyond its boundary, for Green's function and scattering-matrix calculations

The asymptotic completeness of a set of the eigenmodes of an open system with increasing number of modes enables an accurate calculation of the system response in terms of these modes. Using the exact eigenmodes, such completeness is limited to the interior of the system. Here we show that when the eigenmodes of a target system are obtained by the resonant-state expansion, using the modes of a basis system embedding the target system, the completeness extends beyond the boundary of the target system. We illustrate this by using the Mittag-Leffler series of the Green's function expressed in terms of the eigenmodes, which converges to the correct solution anywhere within the basis system, including the space outside the target system. Importantly, this property allows one to treat pertubations outside the target system and to calculate the scattering cross-section using the boundary conditions for the basis system. Choosing a basis system of spherical geometry, these boundary conditions have simple analytical expressions, allowing for an efficient calculation of the response of the target system, as we demonstrate for a resonator in a form of a finite dielectric cylinder.

physics.optics↗

Quantitatively linking morphology and optical response of individual silver nanohedra

The optical response of metal nanoparticles is governed by plasmonic resonances, which are dictated by the particle morphology. A thorough understanding of the link between morphology and optical response requires quantitatively measuring optical and structural properties of the same particle. Here we present such a study, correlating electron tomography and optical micro-spectroscopy. The optical measurements determine the scattering and absorption cross-section spectra in absolute units, and electron tomography determines the 3D morphology. Numerical simulations of the spectra for the individual particle geometry, and the specific optical setup used, allow for a quantitative comparison including the cross-section magnitude. Silver nanoparticles produced by photochemically driven colloidal synthesis, including decahedra, tetrahedra and bi-tetrahedra are investigated. A mismatch of measured and simulated spectra is found when assuming pure silver particles, which is resolved by the presence of a few atomic layers of tarnish on the surface, not evident in electron tomography. The presented method tightens the link between particle morphology and optical response, supporting the predictive design of plasmonic nanomaterials.

physics.optics↗

First-order perturbation theory of eigenmodes for systems with interfaces

We present an exact first-order perturbation theory for the eigenmodes in systems with interfaces causing material discontinuities. We show that when interfaces deform, higher-order terms of the perturbation series can contribute to the eigenmode frequencies in first order in the deformation depth. This means that the usual diagonal approximation is not necessarily equal to the firstorder approximation, rendering the well known single-mode result insufficient. Extracting the true first-order correction from all higher-order terms enables us to recover the diagonal formalism in a modified form. A general formula for the single-mode first-order correction to electromagnetic eigenmodes is derived, capable of treating dispersive, magnetic, and chiral materials with arbitrary shapes.

physics.optics↗

Optical resonances in graded index spheres: A resonant-state expansion study and analytic approximations

Recent improvements in the resonant-state expansion (RSE), focusing on the static mode contribution, have made it possible to treat transverse-magnetic (TM) modes of a spherically symmetric system with the same efficiency as their transverse-electric (TE) counterparts. We demonstrate here that the efficient inclusion of static modes in the RSE results in its quick convergence to the exact solution regardless of the static mode set used. We then apply the RSE to spherically symmetric systems with continuous radial variations of the permittivity. We show that in TM polarization, the spectral transition from whispering gallery to Fabry-Perot modes is characterized by a peak in the mode losses and an additional mode as compared to TE polarization. Both features are explained quantitatively by the Brewster angle of the surface reflection which occurs in this frequency range. Eliminating the discontinuity at the sphere surface by using linear or quadratic profiles of the permittivity modifies this peak and increases the Fabry-Perot mode losses, in qualitative agreement with a reduced surface reflectivity. These profiles also provide a nearly parabolic confinement for the whispering gallery modes, for which an analytical approximation using the Morse potential is presented. Both profiles result in a reduced TE-TM splitting, which is shown to be further suppressed by choosing a profile radially extending the mode fields. Based on the concepts of ray optics, phase analysis of the secular equation, and effective quantum-mechanical potential for a wave equation, we have further developed a number of useful approximations which shed light on the physical phenomena observed in the spectra of graded-index systems.

physics.optics↗