arXiv subjects

Christos Tserkezis

Publications and source records attributed to Christos Tserkezis.

At least 37 records · Page 2Linked to original sources

arXiv2024

Electron beams traversing spherical nanoparticles: analytic and numerical treatment

We present an analytic, Mie theory-based solution for the energy-loss and the photon-emission probabilities in the interaction of spherical nanoparticles with electrons passing nearby and through them, in both cathodoluminescence and electron energy-loss spectroscopies. In particular, we focus on the case of penetrating electron trajectories, for which the complete fully electrodynamic and relativistic formalism has not been reported as yet. We exhibit the efficiency of this method in describing collective excitations in matter through calculations for a dispersive and lossy system, namely a sphere described by a Drude permittivity. Subsequently, we use the analytic solution to corroborate the implementation of electron-beam sources in a state-of-the-art numerical method for problems in electrodynamics, the discontinuous Galerkin time-domain (DGTD) method. We show that the two approaches produce spectra in good mutual agreement, and demonstrate the versatility of DGTD via simulations of spherical nanoparticles characterized by surface roughness. The possibility of simultaneously employing both kinds of calculations (analytic and numerical) facilitates a better understanding of the rich optical response of nanophotonic architectures excited by fast electron beams.

cond-mat.mes-hall↗

arXiv2023

Quantum-informed plasmonics for strong coupling: the role of electron spill-out

The effect of nonlocality on the optical response of metals lies at the forefront of research in nanoscale physics and, in particular, quantum plasmonics. In alkali metals, nonlocality manifests predominantly as electron density spill-out at the metal boundary, and as surface-enabled Landau damping. For an accurate description of plasmonic modes, these effects need be taken into account in the theoretical modelling of the material. The resulting modal frequency shifts and broadening become particularly relevant when dealing with the strong interaction between plasmons and excitons, where hybrid modes emerge and the way they are affected can reflect modifications of the coupling strength. Both nonlocal phenomena can be incorporated in the classical local theory by applying a surface-response formalism embodied by the Feibelman parameters. Here, we implement surface-response corrections in Mie theory to study the optical response of spherical plasmonic--excitonic composites in core--shell configurations. We investigate sodium, a jellium metal dominated by spill-out, for which it has been anticipated that nonlocal corrections should lead to an observable change in the coupling strength, appearing as a modification of the width of the mode splitting. We show that, contrary to expectations, the influence of nonlocality on the anticrossing is minimal, thus validating the accuracy of the local response approximation in strong-coupling photonics.

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arXiv2023

Self-hybridisation between interband transitions and Mie modes in dielectric nanoparticles

We discuss the possibility of self-hybridisation in high-index dielectric nanoparticles, where Mie modes of electric or magnetic type can couple to the interband transitions of the material, leading to spectral anticrossings. Starting with an idealised system described by moderately high constant permittivity with a narrow Lorentzian, in which self-hybridisation is visible for both plane-wave and electron-beam excitation, we embark on a quest for realistic systems where this effect should be visible. We explore a variety of spherical particles made of traditional semiconductors such as Si, GaAs, and GaP. With the effect hardly discernible, we identify two major causes hindering observation of self-hybridisation: the very broad spectral fingerprints of interband transitions in most candidate materials, and the significant overlap between electric and magnetic Mie modes in nanospheres. We thus depart from the spherical shape, and show that interband--Mie hybridisation is indeed feasible in the example of GaAs cylinders, even with a simple plane-wave source. This so-far unreported kind of polariton has to be considered when interpreting experimental spectra of Mie-resonant nanoparticles and assigning modal characters to specific features. On the other hand, it has the potential to be useful for the characterisation of the optical properties of dielectric materials, through control of the hybridisation strength via nanoparticle size and shape.

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arXiv2023

A Dedicated Modelling Scheme for Nonclassical Optical Response from the Nanosphere-on-Mirror Structure

Within the framework of the T-matrix method, we present a modeling tool that predicts the optical response from the Nanosphere-on-Mirror (NSoM) construct. The nonclassical effects in metals are accounted for by the nonlocal hydrodynamic Drude model (NLHDM) or the surface response model (SRM). Two essential elements in the T-matrix method, i.e., the T-matrix of the sphere and the R matrix accounting for the effects of the mirror, have been fully upgraded to include longitudinal waves for the NLHDM and the augmented interface conditions for the SRM. The proposed tool is quantitatively validated both in the near and the far field by an in-house developed BEM solver for the NLHDM where the gap between the sphere and the mirror is as small as 1 nm. Two physical checks are performed, where the results from the classical local response model are compared with the ones from the NLHDM and the SRM. The observed shifts in resonances and reduced field enhancements in the gap region agree well with previous physical findings. The proposed tool may not only serve as a reference tool for other numerical methods, but also provides an ideal platform for investigating nonclassical optical processes in the NSoM, hence paving a semi-analytical way to understand the extreme optics at very small scales.

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arXiv2023

The Uniqueness Theorem for Nonlocal Hydrodynamic Media

We investigate a fundamental electromagnetic theorem, namely the uniqueness theorem, in the context of nonlocal electromagnetics, as simulated by a popular semiclassical model, the Hydrodynamic Drude Model (HDM) and extensions thereof such as the Generalized Nonlocal Optical Response (GNOR). The derivations and proofs presented here give a theoretical foundation to the use of the Additional Boundary Conditions (ABCs), whose necessity is recognized and underlined in virtually all implementations and applications of HDM. Our proofs follow a mathematically relaxed style, borrowing from the literature of established electromagnetics textbooks that study the matter from an engineering perspective. Through this simpler route we deduce clear and intuitive material-response requirements for uniqueness to hold, while using a familiar parlance in a topic that is mostly studied through a physics perspective. Two numerical examples that examine the problem from either a semianalytical or a purely numerical viewpoint support our findings.

physics.app-ph↗

arXiv2023

Nonlocal effects in atom-plasmon interactions

Nonlocal and quantum mechanical phenomena in noble metal nanostructures become increasingly crucial when the relevant length scales in hybrid nanostructures reach the few-nanometer regime. In practice, such mesoscopic effects at metal-dielectric interfaces can be described using exemplary surface-response functions (SRFs) embodied by the Feibelman $d$-parameters. Here we show that SRFs dramatically influence quantum electrodynamic phenomena -- such as the Purcell enhancement and Lamb shift -- for quantum emitters close to a diverse range of noble metal nanostructures interfacing different homogeneous media. Dielectric environments with higher permittivities are shown to increase the magnitude of SRFs calculated within the specular-reflection model. In parallel, the role of SRFs is enhanced in nanostructures characterized by large surface-to-volume ratios, such as thin planar metallic films or shells of core-shell nanoparticles. By investigating emitter quantum dynamics close to such plasmonic architectures, we show that decreasing the width of the metal region, or increasing the permittivity of the interfacing dielectric, leads to a significant change in the Purcell enhancement, Lamb shift, and visible far-field spontaneous emission spectrum, as an immediate consequence of SRFs. We anticipate that fitting the theoretically modelled spectra to experiments could allow for experimental determination of the $d$-parameters.

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arXiv2023

Gain-compensated cavities for the dynamic control of light-matter interactions

We propose an efficient approach for actively controlling the Rabi oscillations in emitter-cavity hybrids based on the presence of an element with optical gain. Inspired by recent developments in parity-time ($\mathcal{PT}$)-symmetry photonics, we show that nano- or micro-cavities where intrinsic losses are partially or fully compensated by an externally controllable amount of gain offer unique capabilities for manipulating the dynamics of emitters. In particular, one can drastically modify the dynamics of the system, increase the overall occupation numbers, enhance the longevity of the Rabi oscillations, and even decelerate them to the point where their experimental observation becomes less challenging. Furthermore, we show that there is a specific gain value that leads to an exceptional point, where both emitter and cavity occupation oscillate practically in phase, with occupation numbers that can significantly exceed unity. By revisiting a recently-introduced Rabi-visibility measure, we provide robust guidelines for quantifying the coupling strength and achieving strong-coupling with adaptable Rabi frequency via loss compensation.

physics.optics↗

arXiv2022

Reconfigurable chirality with achiral excitonic materials in the strong-coupling regime

We introduce and theoretically analyze the concept of manipulating optical chirality via strong coupling of the optical modes of chiral nanostructures with excitonic transitions in molecular layers or semiconductors. With chirality being omnipresent in chemistry and biomedicine, and highly desirable for technological applications related to efficient light manipulation, the design of nanophotonic architectures that sense the handedness of molecules or generate the desired light polarization in an externally controllable manner is of major interdisciplinary importance. Here we propose that such capabilities can be provided by the mode splitting resulting from polaritonic hybridization. Starting with an object with well-known chiroptical response -- here, for a proof of concept, a chiral sphere -- we show that strong coupling with a nearby excitonic material generates two distinct frequency regions that retain the object's chirality density and handedness, which manifest most clearly through anticrossings in circular-dichroism or differential-scattering dispersion diagrams. These windows can be controlled by the intrinsic properties of the excitonic layer and the strength of the interaction, enabling thus the post-fabrication manipulation of optical chirality. Our findings are further verified via simulations of the circular dichroism of a realistic chiral architecture, namely a helical assembly of plasmonic nanospheres embedded in a resonant matrix.

physics.optics↗

arXiv2022

Disentangling cathodoluminescence spectra in nanophotonics: particle eigenmodes vs transition radiation

Cathodoluminescence spectroscopy performed in an electron microscope has proven a versatile tool for analysing the near- and far-field optical response of plasmonic and dielectric nanostructures. Nevertheless, the transition radiation produced by electron impact is often disregarded in the interpretation of the spectra recorded from resonant nanoparticles. Here we show, experimentally and theoretically, that transition radiation can by itself generate distinct resonances which, depending on the time of flight of the electron beam inside the particle, can result from constructive or destructive interference in time. Superimposed on the eigenmodes of the investigated structures, these resonances can distort the recorded spectrum and lead to potentially erroneous assignment of modal characters to the spectral features. We develop an intuitive analogy that helps distinguish between the two contributions. As an example, we focus on the case of silicon nanospheres, and show that our analysis facilitates the unambiguous interpretation of experimental measurements on Mie-resonant nanoparticles.

cond-mat.mes-hall↗

arXiv2022

Fundamental issues with light propagation through $\mathcal{PT}$-symmetric systems

We analyse the emergence of unphysical superluminal group velocities in Su--Schrieffer--Heeger (SSH) parity-time ($\mathcal{PT}$) symmetric chains, and explore the origins of such a behaviour. By comparing the band structure of an infinite loss-gain SSH chain with that of a one-dimensional Bragg stack, we first exclude insufficient coupling consideration in the tight-binding description as the cause of group-velocity divergence. We then focus on material dispersion, and show that indeed, restoring causality in the description of both the lossy and the gain components resolves the problem and recovers finite group velocities, whose real part can only exceed the speed of light in vacuum when accompanied by a significant imaginary part. Our analysis introduces thus the required practical limits in the performance of common $\mathcal{PT}$-symmetric systems.

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arXiv2021

Surface-response functions obtained from equilibrium electron-density profiles

Surface-response functions are one of the most promising routes for bridging the gap between fully quantum-mechanical calculations and phenomenological models in quantum nanoplasmonics. Within all the currently available recipes for obtaining such response functions, \emph{ab initio} calculations remain one of the most predominant, wherein the surface-response function are retrieved via the metal's non-equilibrium response to an external perturbation. Here, we present a complementary approach where one of the most appealing surface-response functions, namely the Feibelman $d$-parameters, yield a finite contribution even in the case where they are calculated directly from the equilibrium properties described under the local-response approximation (LRA), but with a spatially varying equilibrium electron density. Using model calculations that mimic both spill-in and spill-out of the equilibrium electron density, we show that the obtained $d$-parameters are in qualitative agreement with more elaborate, but also more computationally demanding, \emph{ab initio} methods. The analytical work presented here illustrates how microscopic surface-response functions can emerge out of entirely local electrodynamic considerations.

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arXiv2020

Manipulating the photonic Hall effect with hybrid Mie-exciton resonances

We examine the far-field optical response, under-plane wave excitation in the presence of a static magnetic field, of core-shell nanoparticles involving a gyroelectric component, either as the inner or the outer layer, through analytic calculations based on appropriately extended Mie theory. We focus on absorption and scattering of light by bismuth-substituted yttrium iron garnet (Bi:YIG) nanospheres and nanoshells, combined with excitonic materials such as organic-molecule aggregates or two-dimensional transition-metal dichalcogenides, and discuss the hybrid character of the modes emerging from the coupling of the two constituents. We observe the excitation of strong magneto-optic phenomena and explore, in particular, the response and tunability of a magneto-transverse light current, indicative of the photonic Hall effect. We show how interaction between the Bi:YIG and excitonic layers leads to a pair of narrow bands of highly directional scattering, emerging from the aforementioned hybridization, which can be tuned at will by adjusting the geometrical or optical parameters of the system. Our theoretical study introduces optically anisotropic media as promising templates for strong coupling in nanophotonics, offering a means to combine tunable magnetic and optical properties, with potential implications both in the design of all-dielectric photonic devices but also in novel clinical applications.

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arXiv2020

Atomically Thin Boron Nitride as an Ideal Spacer for Metal-Enhanced Fluorescence

The metal-enhanced fluorescence (MEF) considerably enhances the luminescence for various applications, but its performance largely depends on the dielectric spacer between the fluorophore and plasmonic system. It is still challenging to produce a defect-free spacer having an optimized thickness with a subnanometer accuracy that enables reusability without affecting the enhancement. In this study, we demonstrate the use of atomically thin hexagonal boron nitride (BN) as an ideal MEF spacer owing to its multifold advantages over the traditional dielectric thin films. With rhodamine 6G as a representative fluorophore, it largely improves the enhancement factor (up to ~95+-5), sensitivity (10^-8 M), reproducibility, and reusability (~90% of the plasmonic activity is retained after 30 cycles of heating at 350 °C in air) of MEF. This can be attributed to its two-dimensional structure, thickness control at the atomic level, defect-free quality, high affinities to aromatic fluorophores, good thermal stability, and excellent impermeability. The atomically thin BN spacers could increase the use of MEF in different fields and industries.

physics.app-ph↗

arXiv2020

Role of diffusive surface scattering in nonlocal plasmonics

The recent generalised nonlocal optical response (GNOR) theory for plasmonics is analysed, and its main input parameter, namely the complex hydrodynamic convection-diffusion constant, is quantified in terms of enhanced Landau damping due to diffusive surface scattering of electrons at the surface of the metal. GNOR has been successful in describing plasmon damping effects, in addition to the frequency shifts originating from induced-charge screening, through a phenomenological electron diffusion term implemented into the traditional hydrodynamic Drude model of nonlocal plasmonics. Nevertheless, its microscopic derivation and justification is still missing. Here we discuss how the inclusion of a diffusion-like term in standard hydrodynamics can serve as an efficient vehicle to describe Landau damping without resorting to computationally demanding quantum-mechanical calculations, and establish a direct link between this term and the Feibelman $d$ parameter for the centroid of charge. Our approach provides a recipe to connect the phenomenological fundamental GNOR parameter to a frequency-dependent microscopic surface-response function. We therefore tackle one of the principal limitations of the model, and further elucidate its range of validity and limitations, thus facilitating its proper application in the framework of nonclassical plasmonics.

cond-mat.mes-hall↗

arXiv2020

Monitoring strong coupling in nonlocal plasmonics with electron spectroscopies

Plasmon-exciton polaritons provide exciting possibilities to control light-matter interactions at the nanoscale by enabling closer investigation of quantum optical effects and facilitating novel technologies based, for instance, on Bose-Einstein condensation and polaritonic lasing. Nevertheless, observing and visualising polaritons is challenging, and traditional optical microscopy techniques often lead to ambiguities regarding the emergence and strength of the plasmon-exciton coupling. Electron microscopy offers a more robust means to study and verify the nature of plexcitons, but is still hindered by instrument limitations and resolution. A simple theoretical description of electron beam-excited plexcitons is therefore vital to complement ongoing experimental efforts. Here we apply analytic solutions for the electron-loss and photon-emission probabilities to evaluate plasmon-exciton coupling studied either with the recently adopted technique of electron energy-loss spectroscopy, or with the so-far unexplored in this context cathodoluminescence spectroscopy. Foreseeing the necessity to account for quantum corrections in the plasmonic response, we extend these solutions within the framework of general nonlocal hydrodynamic descriptions. As a specific example we study core-shell spherical emitter-molecule hybrids, going beyond the standard local-response approximation through the hydrodynamic Drude model for screening and the generalised nonlocal optical response theory for nonlocal damping. We show that electron microscopies are extremely powerful in describing the interaction of emitters with the otherwise weakly excited by optical means higher-order plasmonic multipoles, a response that survives when quantum-informed models are considered.

cond-mat.mes-hall↗

arXiv2019

Magnetic and Electric Mie-Exciton Polaritons in Silicon Nanodisks

Light-matter interactions at the nanoscale constitute a fundamental ingredient for engineering applications in nanophotonics and quantum optics. To this regard electromagnetic Mie resonances excited in high-refractive index dielectric nanoparticles have recently attracted interest because of their lower losses and better control over the scattering patterns compared to their plasmonic metallic counterparts. The emergence of several resonances in those systems results in an overall high complexity, where the electric and magnetic dipoles have significant overlap in the case of spherical symmetry, thus concealing the contributions of each resonance separately. Here we show, experimentally and theoretically, the emergence of strong light-matter coupling between the magnetic and electric-dipole resonances of individual silicon nanodisks coupled to a J-aggregated organic semiconductor resonating at optical frequencies, evidencing how the different properties of the two resonances results in two different coupling strengths. The energy splittings observed are of the same order of magnitude as in similar plasmonic systems, thus confirming dielectric nanoparticles as promising alternatives for localized strong coupling studies. The coupling of both the electric and magnetic dipole resonances can offer interesting possibilities for the control of directional light scattering in the strong-coupling regime and the dynamic tuning of nanoscale light-matter coupled states by external fields.

physics.optics↗

arXiv2019

On the time evolution at a fluctuating exceptional point

We theoretically evaluate the impact of drift-free noise on the dynamics of $\mathcal{PT}$-symmetric non-Hermitian systems with an exceptional point, which have recently been proposed for sensors. Such systems are currently considered as promising templates for sensing applications, because of their intrinsically extremely sensitive response to external perturbations. However, this applies equally to the impact of fabrication imperfections and fluctuations in the system parameters. Here we focus on the influence of such fluctuations caused by inevitable (thermal) noise and show that the exceptional-point eigenstate is not stable in its presence. To this end, we derive an effective differential equation for the mean time evolution operator averaged over all realizations of the noise field and via numerical analysis we find that the presence of noise leads to exponential divergence of any initial state after some characteristic period of time. We therefore show that it is rather demanding to design sensor systems based on continuous operation at an exceptional point.

physics.optics↗

arXiv2019

Enhanced ponderomotive force in graphene due to interband resonance

We analyze intrinsic nonlinearities in two-dimensional polaritonic materials interacting with an optical wave. Focusing on the case of graphene, we show that the second-order nonlinear optical conductivity due to carrier density fluctuations associated with the excitation of a plasmon polariton is closely related to the ponderomotive force due to the oscillating optical field. This relation is first established through an elegant thermodynamic approach for a Drude-like plasma, in the frequency range where intraband scattering is the dominant contribution to conductivity. Subsequently, we extend our analysis to the interband regime, and show that for energies approximately half the Fermi energy, the intraband contribution to the ponderomotive force diverges. In practice, thermal broadening regularizes this divergence as one would expect, but even at room temperature typically leaves a strong ponderomotive enhancement. Finally, we study the impact of nonlocal corrections and find that nonlocality does not lead to further broadening (as one would expect in the case of Landau damping), but rather to a splitting of the ponderomotive interband resonance. Our analysis should prove useful to the open quest for exploiting nonlinearities in graphene and other two-dimensional polaritonic materials, through effects such as second harmonic generation and photon drag.

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