arXiv subjects

N. Asger Mortensen

Publications and source records attributed to N. Asger Mortensen.

At least 127 records · Page 7Linked to original sources

arXiv2014

Localized plasmons in graphene-coated nanospheres

We present an analytical derivation of the electromagnetic response of a spherical object coated by a conductive film, here exemplified by a graphene coating. Applying the framework of Mie-Lorenz theory augmented to account for a conductive boundary condition, we derive the multipole scattering coefficients, modified essentially through the inclusion of an additive correction in numerator and denominator. By reductionist means, starting from the retarded response, we offer simple results in the quasistatic regime by analyzing the multipolar polarizability and associated dispersion equation for the localized plasmons. We consider graphene coatings of both dielectric and conducting spheres, where in the former case the graphene coating introduces the plasmons and in the latter case modifies in interesting ways the existing ones. Finally, we discuss our analytical results in the context of extinction cross-section and local density of states. Recent demonstrations of fabricated spherical graphene nanostructures make our study directly relevant to experiments.

cond-mat.mes-hall↗

arXiv2014

Nonlocal optical response in metallic nanostructures

This review provides a broad overview of the studies and effects of nonlocal response in metallic nanostructures. In particular, we thoroughly present the nonlocal hydrodynamic model and the recently introduced generalized nonlocal optical response (GNOR) model. The influence of nonlocal response on plasmonic excitations is studied in key metallic geometries, such as spheres and dimers, and we derive new consequences due to the GNOR model. Finally, we propose several trajectories for future work on nonlocal response, including experimental setups that may unveil further effects of nonlocal response.

physics.optics↗

arXiv2014

Plasmonic eigenmodes in individual and bow-tie graphene nanotriangles

Serving as a new two-dimensional plasmonic material, graphene has stimulated an intensive study of its optical properties which benefit from the unique electronic band structure of the underlying honeycomb lattice of carbon atoms. In classical electrodynamics, nanostructured graphene is commonly modeled by the computationally demanding problem of a three-dimensional conducting film of atomic-scale thickness. Here, we propose an efficient alternative two-dimensional electrostatic approach where all the calculation procedures are restricted to the plane of the graphene sheet. To explore possible quantum effects, we perform tight-binding calculations, adopting a random-phase approximation. We investigate the multiple plasmon modes in triangles of graphene, treating the optical response classically as well as quantum mechanically in the case of both armchair and zigzag edge termination of the underlying atomic lattice. Compared to the classical plasmonic spectrum which is "blind" to the edge termination, we find that the quantum plasmon frequencies exhibit blueshifts in the case of armchair edge termination, while redshifts are found for zigzag edges. Furthermore, we find spectral features in the zigzag case which are associated with electronic edge states not present for armchair termination. Merging pairs of such triangles into dimers, the plasmon hybridization leads to energy splitting in accordance with plasmon-hybridization theory, with a lower energy for the antisymmetric modes and a smaller splitting for modes with less confinement to the gap region. The hybridization appears strongest in classical calculations while the splitting is lower for armchair edges and even more reduced for zigzag edges. Our various results illustrate a surprising phenomenon: Even 20 nm large graphene structures clearly exhibit quantum plasmonic features due to atomic-scale details in the edge termination.

cond-mat.mes-hall↗

arXiv2014

Classical and Quantum Plasmonics in Graphene Nanodisks: the Role of Edge States

Edge states are ubiquitous for many condensed matter systems with multicomponent wave functions. For example, edge states play a crucial role in transport in zigzag graphene nanoribbons. Here, we report microscopic calculations of quantum plasmonics in doped graphene nanodisks with zigzag edges. We express the nanodisk conductivity $σ(ω)$ as a sum of the conventional bulk conductivity $σ_{\scriptscriptstyle\text{B}}(ω)$, and a novel term $σ_{\scriptscriptstyle\text{E}}(ω)$, corresponding to a coupling between the edge and bulk states. We show that the edge states give rise to a red-shift and broadening of the plasmon resonance, and that they often significantly impact the absorption efficiency. We further develop simplified models, incorporating nonlocal response within a hydrodynamical approach, which allow a semiquantitative description of plasmonics in the ultrasmall size regime. However, the polarization dependence is only given by fully microscopic models. The approach developed here should have many applications in other systems supporting edge states.

cond-mat.mes-hall↗

arXiv2014

Nonlocal study of ultimate plasmon hybridization

Within our recently proposed generalized nonlocal optical response (GNOR) model, we revisit the fundamental problem of an optically excited plasmonic dimer. The dimer consists of two identical cylinders separated by a nanometre-sized gap. We consider the transition from separated dimers via touching dimers to finally overlapping dimers. In particular, we focus on the touching case, showing a fundamental limit on the hybridization of the bonding plasmon modes due to nonlocality. Using transformation optics we determine a simple analytical equation for the resonance energies of the bonding plasmon modes of the touching dimer.

physics.optics↗

arXiv2014

Nonlocal Response of Metallic Nanospheres Probed by Light, Electrons, and Atoms

Inspired by recent measurements on individual metallic nanospheres that can not be explained with traditional classical electrodynamics, we theoretically investigate the effects of nonlocal response by metallic nanospheres in three distinct settings: atomic spontaneous emission, electron energy loss spectroscopy, and light scattering. These constitute two near-field and one far-field measurements, with zero-, one-, and two-dimensional excitation sources, respectively. We search for the clearest signatures of hydrodynamic pressure waves in nanospheres. We employ a linearized hydrodynamic model and Mie-Lorenz theory is applied for each case. Nonlocal response shows its mark in all three configurations, but for the two near-field measurements we predict especially pronounced nonlocal effects that are not exhibited in far-field measurements. Associated with every multipole order is not only a single blueshifted surface plasmon, but also an infinite series of bulk plasmons that has no counterpart in a local-response approximation. We show that these increasingly blueshifted multipole plasmons become spectrally more prominent at shorter probe-to-surface separations and for decreasing nanosphere radii. For selected metals we predict hydrodynamic multipolar plasmons to be measurable on single nanospheres.

cond-mat.mes-hall↗

arXiv2013

Generalized nonlocal optical response in nanoplasmonics

Metallic nanostructures exhibit a multitude of optical resonances associated with localized surface plasmon excitations. Recent observations of plasmonic phenomena at the sub-nanometer to atomic scale have stimulated the development of various sophisticated theoretical approaches for their description. Here instead we present a comparatively simple semiclassical generalized nonlocal optical response (GNOR) theory that unifies quantum-pressure convection effects and induced-charge diffusion kinetics, with a concomitant complex-valued GNOR parameter. Our theory explains surprisingly well both the frequency shifts and size-dependent damping in individual metallic nanoparticles (MNPs) as well as the observed broadening of the cross-over regime from bonding-dipole plasmons to charge-transfer plasmons in MNP dimers, thus unraveling a classical broadening mechanism that even dominates the widely anticipated short-circuiting by quantum tunneling. We anticipate that the GNOR theory can be successfully applied in plasmonics to a wide class of conducting media, including doped semiconductors and low-dimensional materials such as graphene.

cond-mat.mes-hall↗

arXiv2013

Extremely confined gap surface plasmon modes excited by electrons

High spatial and energy resolution EELS can be employed for detailed characterization of both localized and propagating surface plasmon excitations supported by metal nanostructures, giving insight into fundamental physical phenomena involved in various plasmonic effects. Here, applying EELS to ultra-sharp convex grooves in gold, we directly probe extremely confined gap surface plasmon (GSP) modes excited by swift electrons in nanometer-wide gaps. Both experimental and theoretical EELS data reveal the resonance behavior associated with the excitation of the antisymmetric (with respect to the transverse electric-field component) GSP mode for extremely small gap widths, down to ~5 nm. It is argued that the excitation of this mode, featuring very strong absorption, plays a crucial role in the experimental realization of non-resonant light absorption by ultra-sharp convex grooves with fabrication-induced asymmetry. Occurrence of the antisymmetric GSP mode along with the fundamental GSP mode exploited in plasmonic waveguides with extreme light confinement is a very important factor that should be taken into account in the design of plasmonic nanophotonic circuits and devices.

cond-mat.mes-hall↗

arXiv2013

Plasmon-phonon coupling in large-area graphene dot and antidot arrays

Nanostructured graphene on SiO2 substrates pave the way for enhanced light-matter interactions and explorations of strong plasmon-phonon hybridization in the mid-infrared regime. Unprecedented large-area graphene nanodot and antidot optical arrays are fabricated by nanosphere lithography, with structural control down to the sub-100 nanometer regime. The interaction between graphene plasmon modes and the substrate phonons is experimentally demonstrated and structural control is used to map out the hybridization of plasmons and phonons, showing coupling energies of the order 20 meV. Our findings are further supported by theoretical calculations and numerical simulations.

cond-mat.mes-hall↗

arXiv2013

Absorption and eigenmode calculation for one-dimensional periodic metallic structures using the hydrodynamic approximation

We develop a modal method that solves Maxwell's equations in the presence of the linearized hydrodynamic correction. Using this approach, it is now possible to calculate the full diffraction for structures with period of the order of the plasma wavelength, including not only the transverse but also the longitudinal modes appearing above the plasma frequency. As an example for using this method we solve the diffraction of a plane wave near the plasma frequency from a bi-metallic layer, modeled as a continuous variation of the plasma frequency. We observe absorption oscillations around the plasma frequency. The lower frequency absorption peaks and dips correspond to lowest longitudinal modes concentrated in the lower plasma frequency region. As the frequency is increased, higher order longitudinal modes are excited and extent to the region of higher plasma frequency. Moreover, examination of the propagation constants of these modes reveals that the absorption peaks and dips are directly related to the direction of phase propagation of the longitudinal modes. Furthermore, we formulate a variant of the Plane Wave Expansion method, and used it to calculate the dispersion diagram of such longitudinal modes in a periodically modulated plasma frequency layer.

physics.optics↗

arXiv2013

Green function surface-integral method for nonlocal response of plasmonic nanowires in arbitrary dielectric environments

We develop a nonlocal-response generalization to the Green-function surface-integral method (GSIM), also known as the boundary-element method (BEM). This numerically light method can accurately describe the linear hydrodynamic nonlocal response of arbitrarily shaped plasmonic nanowires in arbitrary dielectric backgrounds. All previous general-purpose methods for nonlocal response are bulk methods. We also expand the possible geometries to which the usual local-response GSIM can be applied, by showing how to regularize singularities that occur in the surface integrals when the nanoparticles touch a dielectric substrate. The same regularization works for nonlocal response. Furthermore, an effective theory is developed to explain the numerically observed nonlocal effects. The nonlocal frequency blueshift of a cylindrical nanowire in an inhomogeneous background generally increases as the nanowire radius and the longitudinal wavenumber become smaller, or when the effective background permittivity or the mode inhomogeneity increase. The inhomogeneity can be expressed in terms of an effective angular momentum of the surface-plasmon mode. We compare local and nonlocal response of free-standing nanowires, and of nanowires close to and on top of planar dielectric substrates. Especially for the latter geometry, considerable differences in extinction cross sections are found for local as compared to nonlocal response, similar to what is found for plasmonic dimer structures.

cond-mat.mes-hall↗

arXiv2013

Blueshift of the surface plasmon resonance in silver nanoparticles: substrate effects

We study the blueshift of the surface plasmon (SP) resonance energy of isolated Ag nanoparticles with decreasing particle diameter, which we recently measured using electron energy loss spectroscopy (EELS). As the particle diameter decreases from 26 down to 3.5 nm, a large blueshift of 0.5 eV of the SP resonance energy is observed. In this paper, we base our theoretical interpretation of our experimental findings on the nonlocal hydrodynamic model, and compare the effect of the substrate on the SP resonance energy to the approach of an effective homogeneous background permittivity. We derive the nonlocal polarizability of a small metal sphere embedded in a homogeneous dielectric environment, leading to the nonlocal generalization of the classical Clausius-Mossotti factor. We also present an exact formalism based on multipole expansions and scattering matrices to determine the optical response of a metal sphere on a dielectric substrate of finite thickness, taking into account retardation and nonlocal effects. We find that the substrate-based calculations show a similar-sized blueshift as calculations based on a sphere in a homogeneous environment, and that they both agree qualitatively with the EELS measurements.

physics.optics↗

arXiv2013

Nonlocal formalism for nanoplasmonics: phenomenological and semi-classical considerations

The plasmon response of metallic nanostructures is anticipated to exhibit nonlocal dynamics of the electron gas when exploring the true nanoscale. We extend the local-response approximation (based on Ohm's law) to account for a general short-range nonlocal response of the homogeneous electron gas. Without specifying further details of the underlying physical mechanism we show how this leads to a Laplacian correction term in the electromagnetic wave equation. Within the hydrodynamic model we demonstrate this explicitly and we identify the characteristic nonlocal range to be vF/omega where vF is the Fermi velocity and omega is the optical angular frequency. For noble metals this gives significant corrections when characteristic device dimensions approach ~1-10 nm, whereas at more macroscopic length scales plasmonic phenomena are well accounted for by the local Drude response.

cond-mat.mes-hall↗

arXiv2013

Broadening of plasmonic resonance due to electron collisions with nanoparticle boundary: quantum-mechanical consideration

We present a quantum mechanical approach to calculate broadening of plasmonic resonances in metallic nanostructures due to collisions of electrons with the surface of the structure. The approach is applicable if the characteristic size of the structure is much larger than the de Broglie electron wavelength in the metal. The approach can be used in studies of plasmonic properties of both single nanoparticles and arrays of nanoparticles.

physics.optics↗

arXiv2013

Hybridization of quantum plasmon modes in coupled nanowires: From the classical to the tunneling regime

We present full quantum mechanical calculations of the hybridized plasmon modes of two nanowires at small separation, providing real space visualization of the modes in the transition from the classical to the quantum tunneling regime. The plasmon modes are obtained as certain eigenfunctions of the dynamical dielectric function which is computed using time dependent density functional theory (TDDFT). For freestanding wires, the energy of both surface and bulk plasmon modes deviate from the classical result for low wire radii and high momentum transfer due to effects of electron spill-out, non-local response, and coupling to single-particle transitions. For the wire dimer the shape of the hybridized plasmon modes are continuously altered with decreasing separation, and below 6 Å the energy dispersion of the modes deviate from classical results due to the onset of weak tunneling. Below 2-3 Å separation this mode is replaced by a charge-transfer plasmon which blue shifts with decreasing separation in agreement with experiment, and marks the onset of the strong tunneling regime.

cond-mat.mes-hall↗

arXiv2013

Enhanced light-matter interaction in graphene-covered gold nanovoid arrays

The combination of graphene with noble-metal nanostructures is currently being explored for strong light-graphene interaction enhanced by plasmons. We introduce a novel hybrid graphene-metal system for studying light-matter interactions with gold-void nanostructures exhibiting resonances in the visible range. Strong coupling of graphene layers to the plasmon modes of the nanovoid arrays results in significant frequency shifts of the underlying plasmon resonances, enabling more than 30% absolute light absorption in a single layer of graphene and up to 700-fold enhancement of the Raman response of the graphene. These new perspectives enable us to verify the presence of graphene on gold-void arrays and the enhancement even allows us to accurately quantify the number of layers. Experimental observations are further supported by numerical simulations and perturbation-theory analysis. The graphene gold-void platform is beneficial for sensing of molecules and placing R6G dye molecules on top of the graphene, we observe a strong enhancement of the R6G Raman fingerprints. These results pave the way toward advanced substrates for surface-enhanced Raman scattering (SERS) with potential for unambiguous single-molecule detection on the atomically well-defined layer of graphene.

cond-mat.mes-hall↗

arXiv2013

Nonlocal response in thin-film waveguides: loss versus nonlocality and breaking of complementarity

We investigate the effects of nonlocal response on the surface-plasmon polariton guiding properties of the metal-insulator (MI), metal-insulator-metal (MIM), and insulator-metal-insulator (IMI) waveguides. The nonlocal effects are described by a linearized hydrodynamic model, which includes the Thomas-Fermi internal kinetic energy of the free electrons in the metal. We derive the nonlocal dispersion relations of the three waveguide structures taking into account also retardation and interband effects, and examine the delicate interplay between nonlocal response and absorption losses in the metal. We also show that nonlocality breaks the complementarity of the MIM and IMI waveguides found in the non-retarded limit.

physics.optics↗

arXiv2013

Experimental observation of plasmons in a graphene monolayer resting on a two-dimensional subwavelength silicon grating

We experimentally demonstrate graphene-plasmon polariton excitation in a continuous graphene monolayer resting on a two-dimensional subwavelength silicon grating. The subwavelength silicon grating is fabricated by a nanosphere lithography technique with a self-assembled nanosphere array as a template. Measured transmission spectra illustrate the excitation of graphene-plasmon polaritons, which is further supported by numerical simulations and theoretical prediction of plasmonband diagrams. Our grating-assisted coupling to graphene-plasmon polaritons forms an important platform for graphene-based opto-electronics applications.

physics.optics↗