arXiv subjects

N. Asger Mortensen

Publications and source records attributed to N. Asger Mortensen.

At least 37 records · Page 2Linked to original sources

arXiv2025

Self-similar plasmonic nanolenses: mesoscopic ensemble averaging and chiral light-matter interactions

We investigate how the near-field enhancement of self-similar nanolenses, made of three plasmonic nanospheres with decreasing sizes and separations, is affected by quantum corrections in the optical response of the metal, and by fabrication imperfections related to the positioning of the spheres in the nanolens. In particular, we integrate mesoscopic phenomena, such as electron spill-in and -out and surface-enabled Landau damping, via the surface-response formalism, focusing particularly on the role of spill-out in alkali metals. In addition, we take realistic imperfections in the nanofabrication process into account, through numerical averaging of both far- and near-field spectra for large collections of nanolenses. Statistical analysis of hundreds of trimers shows that inevitable deviations from the perfectly aligned chain only slightly, if at all, impair the field enhancement, as long as the average misplacement is kept within 1 nm from the ideal situation. Wishing to explore whether such imperfections can be harvested for practical applications, we probe the potential for triggering chiral response. Our results verify that imperfect nanolenses can display considerable light-induced optical activity and circular dichroism, while providing a means to manipulate the optical chirality density. This highlights how promising the nanolensing effect is for chiral light-matter interactions. Nonetheless, we emphasize that quantification of chiral light-matter interactions can be largely affected by mesoscopic phenomena, which cannot be ignored when near-field quantities like optical chirality density are investigated.

cond-mat.mes-hall↗

arXiv2024

Quantum-hydrodynamic modal perspective on plasmonic gap structures

Plasmonic gap structures are among the few configurations capable of generating extreme light confinement, finding applications in surface-enhanced spectroscopy, ultrasensitive detection, photocatalysis and more. Their plasmonic response undergoes a dramatic, quantum effect-driven transition as the gap size approaches zero. Modal analysis can reveal insights into the mechanisms governing this process, which are otherwise obscured by nonlocal damping effects. Here, we offer a fresh modal perspective on the transition of the plasmonic response using quantum hydrodynamic theory (QHT)-based quasinormal mode (QNM) analysis. Focusing on the bonding dipolar and charge-transfer plasmons of a nanosphere dimer, we examine the detailed mode transition through the touching regime as well as the asymptotic behavior compared with the classical results as the constituent nanoparticles either separate or overlap. The complex eigenfrequency particularly provides accurate information on the linewidth and quality factor of the plasmon modes. We introduce an index to characterize charge-transfer efficiency, especially for the charge-transfer plasmon. The significant role of nonlocal damping in the mode evolution is elucidated by our mode-resolved QHT-QNM analysis. The insights from our theoretical study provide an integrated understanding of mode evolution in plasmonic gap structures, which can further advance gap structure-based applications.

cond-mat.mes-hall↗

arXiv2024

Tunable exciton polaritons in band-gap engineered hexagonal boron nitride

We show that hexagonal boron nitride (hBN), a two-dimensional insulator, when subjected to an external superlattice potential forms a new paradigm for electrostatically tunable excitons in the near- and mid-ultraviolet (UV). The imposed potential has three consequences: (i) it renormalizes the effective mass tensor, leading to anisotropic effective masses; (ii) it renormalizes the band gap, eventually reducing it; (iii) it reduces the exciton binding energies. All these consequences depend on a single dimensionless parameter, which includes the product of strength of the external potential with its period. In addition to the excitonic energy levels, we compute the optical conductivity along two orthogonal directions, and from it the absorption spectrum. The results for the latter show that our system is able to mimic a grid polarizer. These characteristics make one-dimensional hBN superlattices a viable and unexplored platform for fine-tuned polaritonics in the UV to visible spectral range.

cond-mat.mes-hall↗

arXiv2024

Direct electrical modulation of surface response in a single plasmonic nanoresonator

Classical electrodynamics describes the optical response of systems using bulk electronic properties and infinitesimally thin boundaries. However, due to the quantum nature of electrons, interfaces have a finite thickness. Non-classical surface effects become increasingly important as ever smaller nanoscale systems are realized and eventually dominate over volume-related phenomena. Investigating the response of surface electrons in such systems, therefore, becomes imperative. One way to gain control over non-classical interface effects and study them is through electrical gating, as the static screening charges reside exclusively at the surface. Here, we investigate the modulation of the surface response upon direct electric charging of a single plasmonic nanoresonator by measuring the resulting changes in resonance. We analyze the observed effects within the general framework of surface-response functions and provide a basic model derived from electron spill-out within the local-response approximation (LRA). Our observed change in resonance frequency is well accounted for by assuming a modulation of the in-plane surface current. Surprisingly, we also measure a change in the resonance width, where adding electrons to the surface leads to a narrowing of the plasmonic resonance, i.e., reduced losses. The description of such effects requires considering nonlocal effects and the inclusion of a possible anisotropy of the perturbed surface permittivity. Our experiment, therefore, opens a vast field of investigations on how to gain control over the surface response in plasmonic resonators and to develop ultrafast and extremely small electrically driven plasmonic modulators and metasurfaces by leveraging electrical control over non-classical surface effects.

physics.optics↗

arXiv2024

Topology in a one-dimensional plasmonic crystal

In this paper we study the topology of the bands of a plasmonic crystal composed of graphene and of a metallic grating. Firstly, we derive a Kronig-Penney type of equation for the plasmonic bands as function of the Bloch wavevector and discuss the propagation of the surface plasmon polaritons on the polaritonic crystal using a transfer-matrix approach considering a finite relaxation time. Second, we reformulate the problem as a tight-binding model that resembles the Su-Schrieffer-Heeger (SSH) Hamiltonian, one difference being that the hopping amplitudes are, in this case, energy dependent. In possession of the tight-binding equations it is a simple task to determine the topology (value of the winding number) of the bands. This allows to determine the existense or absence of topological end modes in the system. Similarly to the SSH model, we show that there is a tunable parameter that induces topological phase transitions from trivial to non-trivial. In our case, it is the distance d between the graphene sheet and the metallic grating. We note that d is a parameter that can be easily tuned experimentally simply by controlling the thickness of the spacer between the grating and the graphene sheet. It is then experimentally feasible to engineer devices with the required topological properties. Finally, we suggest a scattering experiment allowing the observation of the topological states.

cond-mat.mes-hall↗

arXiv2024

Dirac plasmon polaritons and magnetic modes in topological-insulator nanoparticles

We demonstrate the existence of previously unreported magnetic modes with record-high magnetic Purcell factors in topological-insulator nanospheres. Focusing on bismuth selenide (Bi$_{2}$Se$_{3}$), and based on full electromagnetic Mie theory, we find magnetic modes arising from both displacement current loops in the bulk, and surface currents due to delocalized surface states, induced by electronic transitions between topologically protected states within the Dirac cone and discretized due to the sphere finite size. Furthermore, we discuss how Dirac plasmon polaritons, resulting from the interaction between THz photons and Dirac electrons, dramatically influence both the magnetic and the electric transitions of quantum emitters placed near Bi$_2$Se$_3$ nanospheres, significantly enhancing the corresponding Purcell factors. These findings position Bi$_{2}$Se$_{3}$ nanospheres, whose optical response is related to a richness of physical mechanisms, among the most promising candidates for enhancing light--matter interactions in nanophotonics and THz technologies.

cond-mat.mes-hall↗

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↗

arXiv2024

Fourier analysis of near-field patterns generated by propagating polaritons

Scattering-type scanning near-field optical microscope (s-SNOM) has become an essential tool to study polaritons - quasiparticles of light coupled to collective charge oscillations - via direct probing of their near field with a spatial resolution far beyond the diffraction limit. However, extraction of the polariton complex propagation constant from the near-field images requires subtle considerations that have not received necessary attention so far. In this study, we discuss important yet overlooked aspects of the near-field analysis. First, we experimentally demonstrate that the sample orientation inside the s-SNOM may significantly affect the near-field interference pattern of mid-infrared polaritons, leading to an error in momentum measurement up to 7.7% even for the modes with effective index of 12.5. Second, we establish a methodology to correctly extract the polariton damping rate from the interference fringes depending on their origin - the s-SNOM nano-tip or the material edge. Overall, our work provides a unified framework for the accurate extraction of the polariton momentum and damping from the near-field interference fringes.

physics.optics↗

arXiv2024

Scaling behavior of the degree of circular polarization of surface plasmon polariton

Surface plasmon polaritons (SPPs) carry transverse optical spin within the evanescent field, which has enabled the demonstration of various chiral light-matter interactions in classical and quantum systems. To achieve high spin selectivity in the interactions, the elliptical polarization of the evanescent field should be made circular, but the engineering principle of the degree of circular polarization (DOCP) of SPPs has been lacking. In this study, we theoretically and numerically investigate the scaling behavior of the DOCP of the SPP field with respect to the modal effective refractive index (neff). The DOCP of the SPP field exhibits power-law scalability to the effective refractive index in the 1D layered system, regardless of the material, structural geometry, and excitation wavelength. The power-law scalability is also confirmed in 2D waveguide structures for in-plane and out-of-plane SPP fields, but the scaling exponents vary depending on the distance from the waveguide boundaries by the reduced symmetry of the given system. Due to Lorentz reciprocity, the power-law scalability can be extended to the coupling directionality of chiral emitters towards the plasmonic waveguide. To this end, we propose a chiral photonic platform for enhanced light-valley interaction, which utilizes simultaneous enhancement of the DOCP and coupling directionality. An incident SPP can excite a chiral emitter with high spin selectivity that unidirectionally couples the emitted light into the plasmonic waveguide depending on the valley polarization of excitons in 2D material. Our work provides a ground rule for designing chiral nanophotonic systems and paves the way for the exploration of scale-free phenomena of electromagnetic waves.

physics.optics↗

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.

cond-mat.mes-hall↗

arXiv2023

High-index and low-loss topological insulators for mid-infrared nanophotonics

Topological insulators generally have dielectric bulk and conductive surface states. Consequently, some of these materials have been shown to support polaritonic modes at visible and THz frequencies. At the same time, the optical properties of topological insulators in the mid-infrared (IR) remain poorly investigated. We employ near-field imaging to probe the mid-IR response from the exfoliated flakes of bismuth (Bi) / selenide (Se) / telluride (Te) / antimony (Sb) crystals with varying stoichiometry - Bi2Se3, Bi2Te2Se, and Bi1.5Sb0.5Te1.7Se1.3 - in pristine form as well as covered by thin flakes of hexagonal boron nitride (hBN). Contrary to theoretical expectations, all three materials exhibit a dielectric response with a high refractive index and with a loss below the experimental detection limit. Particularly, the near-field mapping of propagating phonon-polaritons in hBN demonstrates that these van der Waals crystals act as a practically lossless dielectric substrate with an ultra-high refractive index of up to 7.5 in Bi2Te2Se. Such a unique dielectric crystal would be of great advantage for numerous nanophotonic applications in the mid-IR.

cond-mat.mtrl-sci↗

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.

cond-mat.mes-hall↗

arXiv2023

Inducing room-temperature valley polarization of excitonic emission in transition metal dichalcogenide monolayers

The lowest energy states in transition metal dichalcogenide (TMD) monolayers follow valley selection rules, which have attracted vast interest due to the possibility of encoding and processing of quantum information. However, these quantum states are strongly affected by the temperature-dependent intervalley scattering causing complete valley depolarization, which is hampering any practical applications of TMD monolayers at room temperature. Therefore, for achieving clear and robust valley polarization in TMD monolayers one needs to suppress parasitic depolarization processes, which is the central challenge in the growing field of valleytronics. Here, in electron-doping experiments on TMD monolayers, we demonstrate that strong doping levels beyond $10^{13}$~cm$^{-2}$ can induce 61\% and 37\% valley contrast at room temperature in tungsten diselenide and molybdenum diselenide monolayers, respectively. Our results indicate that charged excitons in TMD monolayers can be utilized as quantum units in designing of practical valleytronic devices operating at 300 K.

cond-mat.mes-hall↗

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.

cond-mat.mes-hall↗

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↗

arXiv2023

Brobdingnagian photon bunching in cathodoluminescence of excitons in WS$_2$ monolayer

Cathodoluminescence spectroscopy in conjunction with second-order auto-correlation measurements of $g_2(τ)$ allows to extensively study the synchronization of quantum light sources in low-dimensional structures. Co-existing excitons in two-dimensional transition metal dichalcogenide monolayers provide a great source of identical quantum emitters which can be simultaneously excited by an electron. In this article, we demonstrate large photon bunching with $g_2(0)$ up to $156\pm16$ of a tungsten disulfide monolayer, exhibiting a strong dependence on the electron-beam current density. To further improve the excitation synchronization and the electron-emitter interaction, we show exemplary that the careful selection of a simple and compact geometry -- a thin, monocrystalline gold nanodisk -- can be used to realize a record-high bunching $g_2(0)$ of up to $2152\pm236$. This approach to control the electron excitation of excitons in a \ce{WS2} monolayer allows for the synchronization of quantum emitters in an ensemble, which is important to further advance quantum information processing and computing technologies.

cond-mat.mes-hall↗

arXiv2023

Sub-to-super-Poissonian photon statistics in cathodoluminescence of color center ensembles in isolated diamond crystals

Impurity-vacancy centers in diamond offer a new class of robust photon sources with versatile quantum properties. While individual color centers commonly act as single-photon sources, their ensembles have been theoretically predicted to have tunable photon-emission statistics. Importantly, the particular type of excitation affects the emission properties of a color center ensemble within a diamond crystal. While optical excitation favors non-synchronized excitation of color centers within an ensemble, electron-beam excitation can synchronize the emitters and thereby provides a control of the second-order correlation function $g_2(0)$. In this letter, we demonstrate experimentally that the photon stream from an ensemble of color centers can exhibit $g_2(0)$ both above and below unity. Such a photon source based on an ensemble of few color centers in a diamond crystal provides a highly tunable platform for informational technologies operating at room temperature.

cond-mat.mes-hall↗

arXiv2023

Nonlinear photoluminescence in gold thin films

Promising applications in photonics are driven by the ability to fabricate crystal-quality metal thin films of controlled thickness down to a few nanometers. In particular, these materials exhibit a highly nonlinear response to optical fields owing to the induced ultrafast electron dynamics, which is however poorly understood on such mesoscopic length scales. Here, we reveal a new mechanism that controls the nonlinear optical response of thin metallic films, dominated by ultrafast electronic heat transport when the thickness is sufficiently small. By experimentally and theoretically studying electronic transport in such materials, we explain the observed temporal evolution of photoluminescence in pump-probe measurements that we report for crystalline gold flakes. Incorporating a first-principles description of the electronic band structures, we model electronic transport and find that ultrafast thermal dynamics plays a pivotal role in determining the strength and time-dependent characteristics of the nonlinear photoluminescence signal, which is largely influenced by the distribution of hot electrons and holes, subject to diffusion across the film as well as relaxation to lattice modes. Our findings introduce conceptually novel elements triggering the nonlinear optical response of nanoscale materials while suggesting additional ways to control and leverage hot carrier distributions in metallic films.

cond-mat.mes-hall↗