Collective Electronic Excitations Research Articles

Quantum-size effects in the loss function of Pb(111) thin films: An ab initio study

A theoretical study of collective electronic excitations in free-standing Pb(111) thin films consisting of 1--5 monolayers (MLs) and a 21-ML film is presented. The calculations are carried out applying the linear response theory, with full inclusion of the electron band structure by means of a first-principles pseudopotential approach in a supercell scheme. In the case of the thickest film, we find that, due to strong bulklike interband transitions, at the Pb(111) surface there are two surface modes. For thin films, a mechanism of transformation of these modes to the symmetric and antisymmetric classic hybrid plasmons is investigated. Pronounced quantum-size effects on plasmon modes of the thinnest films are found. Strong influence of the band structure on dispersion and lifetime of such modes is demonstrated. The present results are in good agreement with available experimental data for a Pb surface and thin films.

Probing the local nature of excitons and plasmons in few-layer MoS2

Excitons and plasmons are the two most fundamental types of collective electronic excitations occurring in solids. Traditionally, they have been studied separately using bulk techniques that probe their average energetic structure over large spatial regions. However, as the dimensions of materials and devices continue to shrink, it becomes crucial to understand how these excitations depend on local variations in the crystal- and chemical structure on the atomic scale. Here, we use monochromated low-loss scanning-transmission-electron-microscopy electron-energy-loss spectroscopy, providing the best simultaneous energy and spatial resolution achieved to-date to unravel the full set of electronic excitations in few-layer MoS2 nanosheets over a wide energy range. Using first-principles, many-body calculations we confirm the excitonic nature of the peaks at ~ 2 and ~ 3 eV in the experimental electron-energy-loss spectrum and the plasmonic nature of higher energy-loss peaks. We also rationalise the non-trivial dependence of the electron-energy-loss spectrum on beam and sample geometry such as the number of atomic layers and distance to steps and edges. Moreover, we show that the excitonic features are dominated by the long wavelength (q = 0) components of the probing field, while the plasmonic features are sensitive to a much broader range of q-vectors, indicating a qualitative difference in the spatial character of the two types of collective excitations. Our work provides a template protocol for mapping the local nature of electronic excitations that open new possibilities for studying photo-absorption and energy transfer processes on a nanometer scale.

Collective electronic excitation in a trapped ensemble of photogenerated dipolar excitons and free holes revealed by inelastic light scattering

Photogenerated excitonic ensembles confined in coupled GaAs quantum wells are probed by a complementary approach of emission spectroscopy and resonant inelastic light scattering. Lateral electrostatic trap geometries are used to create dense systems of spatially indirect excitons and excess holes with similar densities in the order of 10$^{11}$ cm$^{-2}$. Inelastic light scattering spectra reveal a very sharp low-lying collective mode that is identified at an energy of 0.44 meV and a FWHM of only ~50 $\mu$eV. This mode is interpreted as a plasmon excitation of the excess hole system coupled to the photogenerated indirect excitons. The emission energy of the indirect excitons shifts under the application of a perpendicular applied electric field with the quantum-confined Stark effect unperturbed from the presence of free charge carriers. Our results illustrate the potential of studying low-lying collective excitations in photogenerated exciton systems to explore the many-body phase diagram, related phase transitions, and interaction physics.

Optimization of Nanoparticle-Based SERS Substrates through Large-Scale Realistic Simulations.

Surface-enhanced Raman scattering (SERS) has become a widely used spectroscopic technique for chemical identification, providing unbeaten sensitivity down to the single-molecule level. The amplification of the optical near field produced by collective electron excitations —plasmons— in nanostructured metal surfaces gives rise to a dramatic increase by many orders of magnitude in the Raman scattering intensities from neighboring molecules. This effect strongly depends on the detailed geometry and composition of the plasmon-supporting metallic structures. However, the search for optimized SERS substrates has largely relied on empirical data, due in part to the complexity of the structures, whose simulation becomes prohibitively demanding. In this work, we use state-of-the-art electromagnetic computation techniques to produce predictive simulations for a wide range of nanoparticle-based SERS substrates, including realistic configurations consisting of random arrangements of hundreds of nanoparticles with various morphologies. This allows us to derive rules of thumb for the influence of particle anisotropy and substrate coverage on the obtained SERS enhancement and optimum spectral ranges of operation. Our results provide a solid background to understand and design optimized SERS substrates.

Meta-Optics with Mie Resonances

In nanophotonics, subwavelength localization of light is usually associated with plasmonics, the collective excitation of electrons and electromagnetic waves at metallic surfaces. Recent developments in the physics of high-index dielectric nanoparticles, however, suggest an alternative mechanism of light localization: low-order dipole and higherorder multipole Mie resonances. These resonances can generate a strong magnetic response that can be leveraged in designing metasurfaces with unidirectional scattering, as well as efficient metadevices. Indeed, as the power of this approach becomes increasingly apparent, high-index nanomaterials could complement, or even substitute for, plasmonic materials in a range of devices—and could spur a new era in nonlinear nanophotonics.

Subwavelength electromagnetics below the diffraction limit

As a fundamental property of waves, diffraction plays an important role in many physical problems. However, diffraction makes waves in free space unable to be focused into an arbitrarily small space, setting a fundamental limit (the so-called diffraction limit) to applications such as imaging, lithography, optical recording and waveguiding, etc. Although the diffraction effect can be suppressed by increasing the refractive index of the surrounding medium in which the electromagnetic and optical waves propagate, such a technology is restricted by the fact that natural medium has a limited refractive index. In the past decades, surface plasmon polaritons (SPPs) have received special attention, owing to its ability to break through the diffraction limit by shrinking the effective wavelength in the form of collective excitation of free electrons. By combining the short wavelength property of SPPs and subwavelength structure in the two-dimensional space, many exotic optical effects, such as extraordinary light transmission and optical spin Hall effect have been discovered and utilized to realize functionalities that control the electromagnetic characteristics (amplitudes, phases, and polarizations etc.) on demand. Based on SPPs and artificial subwavelength structures, a new discipline called subwavelength electromagnetics emerged in recent years, thus opening a door for the next-generation integrated and miniaturized electromagnetic and optical devices and systems. In this paper, we review the theories and methods used to break through the diffraction limit by briefly introducing the history from the viewpoint of electromagnetic optics. It is shown that by constructing plasmonic metamaterials and metasurfaces on a subwavelength scale, one can realize the localized phase modulation and broadband dispersion engineering, which could surpass many limits of traditional theory and lay the basis of high-performance electromagnetic and optical functional devices. For instance, by constructing gradient phase on the metasurfaces, the traditional laws of reflection and refraction can be rewritten, while the electromagnetic and geometric shapes could be decoupled, both of which are essential for realizing the planar and conformal lenses and other functional devices. At the end of this paper, we discuss the future development trends of subwavelength electromagnetics. Based on the fact that different concepts, such as plasmonics, metamaterials and photonic crystals, are closely related to each other on a subwavelength scale, we think, the future advancements and even revolutions in subwavelength electromagnetics may rise from the in-depth intersection of physical, chemical and even biological areas. Additionally, we envision that the material genome initiative can be borrowed to promote the information exchange between different engineering and scientific teams and to enable the fast designing and implementing of subwavelength structured materials.

Dielectronic recombination rate in statistical model

The dielectronic recombination rate of multielectron ions was calculated by means of the statistical approach. It is based on an idea of collective excitations of atomic electrons with the local plasma frequencies. These frequencies are expressed via the Thomas-Fermi model electron density distribution. The statistical approach provides fast computation of DR rates that are compared with the modern quantum mechanical calculations. The results are important for current studies of thermonuclear plasmas with the tungsten impurities.

Temperature effect on acoustic plasmons

The presence of several kinds of carriers at the Fermi surface results in interesting complex dielectric properties of the bulk Pd in the low-energy excitation range. A most spectacular manifestation of this is the presence of a collective electronic excitation characterized by a soundlike dispersion, termed acoustic plasmon (AP). Due to the characteristic dispersion reaching zero energy in the long-wavelength limit, the question of the thermal stability of the excitation spectrum arises. In this work we explore this problem investigating the thermal effect on the electronic excitation spectrum in this material, tracing how the AP properties vary with the temperature increase. The main effect consists in the gradual destruction of AP in the energy range corresponding to the temperature.

Photoionization of multishell fullerenes studied by ab initio and model approaches*

Photoionization of two buckyonions, C60@C240 and C20@C60, is investigated by means of time-dependent density-functional theory (TDDFT). The TDDFT-based photoabsorption spectrum of C60@C240, calculated in a broad photon energy range, resembles the sum of spectra of the two isolated fullerenes, thus illustrating the absence of strong plasmonic coupling between the fullerenes which was proposed earlier. The calculated spectrum of the smaller buckyonion, C20@C60, differs significantly from the sum of the cross sections of the individual fullerenes because of strong geometrical distortion of the system. The contribution of collective electron excitations arising in individual fullerenes is evaluated by means of plasmon resonance approximation (PRA). An extension of the PRA formalism is presented, which allows for the study of collective electron excitations in multishell fullerenes under photon impact. An advanced analysis of photoionization of buckyonions, performed using modern computational and analytical approaches, provides valuable information on the response of complex molecular systems to the external electromagnetic field.

Nonlinear optical observation of coherent acoustic Dirac plasmons in thin-film topological insulators.

Low-energy collective electronic excitations exhibiting sound-like linear dispersion have been intensively studied both experimentally and theoretically for a long time. However, coherent acoustic plasmon modes appearing in time-domain measurements are rarely observed due to Landau damping by the single-particle continua. Here we report on the observation of coherent acoustic Dirac plasmon (CADP) modes excited in indirectly (electrostatically) opposite-surface coupled films of the topological insulator Bi2Se3. Using transient second-harmonic generation, a technique capable of independently monitoring the in-plane and out-of-plane electron dynamics in the films, the GHz-range oscillations were observed without corresponding oscillations in the transient reflectivity. These oscillations were assigned to the transverse magnetic and transverse electric guided CADP modes induced by the evanescent guided Lamb acoustic waves and remained Landau undamped due to fermion tunnelling between the opposite-surface Dirac states.

Terahertz Spectroscopy of Individual Single-Walled Carbon Nanotubes as a Probe of Luttinger Liquid Physics.

Luttinger liquid theory predicts that collective electron excitations due to strong electron-electron interactions in a one-dimensional (1D) system will result in a modification of the collective charge-propagation velocity. By utilizing a circuit model for an individual metallic single-walled carbon nanotube as a nanotransmission line, it has been shown that the frequency-dependent terahertz impedance of a carbon nanotube can probe this expected 1D Luttinger liquid behavior. We excite terahertz standing-wave resonances on individual antenna-coupled metallic single-walled carbon nanotubes. The terahertz signal is rectified using the nanotube contact nonlinearity, allowing for a low-frequency readout of the coupled terahertz current. The charge velocity on the nanotube is determined from the terahertz spectral response. Our measurements show that a carbon nanotube can behave as a Luttinger liquid system with charge-propagation velocities that are faster than the Fermi velocity. Understanding what determines the charge velocity in low-dimensional conductors is important for the development of next generation nanodevices.

Collective electronic excitations in the ultra violet regime in 2-D and 1-D carbon nanostructures achieved by the addition of foreign atoms.

Plasmons in the visible/UV energy regime have attracted great attention, especially in nano-materials, with regards to applications in opto-electronics and light harvesting; tailored enhancement of such plasmons is of particular interest for prospects in nano-plasmonics. This work demonstrates that it is possible, by adequate doping, to create excitations in the visible/UV regime in nano-carbon materials, i.e., carbon nanotubes and graphene, with choice of suitable ad-atoms and dopants, which are introduced directly into the lattice by low energy ion implantation or added via deposition by evaporation. Investigations as to whether these excitations are of collective nature, i.e., have plasmonic character, are carried out via DFT calculations and experiment-based extraction of the dielectric function. They give evidence of collective excitation behaviour for a number of the introduced impurity species, including K, Ag, B, N, and Pd. It is furthermore demonstrated that such excitations can be concentrated at nano-features, e.g., along nano-holes in graphene through metal atoms adhering to the edges of these holes.

Statistical Model of Dielectronic Recombination of Heavy Ions in Plasmas

AbstractCalculation of the total dielectronic recombination (DR) rates was done in the frame of a statistical model of atoms. The model is based on the idea of collective excitations of atomic electrons with the local plasma frequency, which depends on atomic electrons density distribution. The electron density is described in a frame of the Thomas‐Fermi model of atoms. Simple scaling laws for temperature Te and nuclear charge Z dependences follow from the statistical model of DR. Results of the statistical model were compared with other numerical data following detailed level‐by‐level computations for different multielectron ions. The specific attention is paid to Ni‐like ion sequences of different chemical elements in order to check the Z ‐dependence of DR rates. A comparison with numerical data of Flexible Atomic Code (FAC) is presented for tungsten ions. The reasonable correspondence between the statistical model and the detailed numerical data is demonstrated. The application of the statistical model provides very simple and fast calculations of the DR rates useful in modern plasma modelling. (© 2016 WILEY‐VCH Verlag GmbH & Co. KGaA, Weinheim)

Localized surface plasmon enhanced photothermal conversion in Bi2Se3 topological insulator nanoflowers.

Localized surface plasmons (LSP), the confined collective excitations of electrons in noble metal and doped semiconductor nanostructures, enhance greatly local electric field near the surface of the nanostructures and result in strong optical response. LSPs of ordinary massive electrons have been investigated for a long time and were used as basic ingredient of plasmonics and metamaterials. LSPs of massless Dirac electrons, which could result in novel tunable plasmonic metamaterials in the terahertz and infrared frequency regime, are relatively unexplored. Here we report for first time the observation of LSPs in Bi2Se3 topological insulator hierarchical nanoflowers, which are consisted of a large number of Bi2Se3 nanocrystals. The existence of LSPs can be demonstrated by surface enhanced Raman scattering and absorbance spectra ranging from ultraviolet to near-infrared. LSPs produce an enhanced photothermal effect stimulated by near-infrared laser. The excellent photothermal conversion effect can be ascribed to the existence of topological surface states, and provides us a new way for practical application of topological insulators in nanoscale heat source and cancer therapy.

Two-dimensional crossover and strong coupling of plasmon excitations in arrays of one-dimensional atomic wires

The collective electronic excitations of arrays of Au chains on regularly stepped Si(553) and Si(775) surfaces were studied using electron loss spectroscopy with simultaneous high energy and momentum resolution (ELS-LEED) in combination with low energy electron diffraction (SPA-LEED) and tunneling microscopy. Both surfaces contain a double chain of gold atoms per terrace. Although one-dimensional metallicity and plasmon dispersion is observed only along the wires, two-dimensional effects are important, since plasmon dispersion explicitly depends both on the structural motif of the wires and the terrace width. The electron density on each terrace turns out to be modulated, as seen by tunneling spectroscopy (STS). The effective wire width of 7.5\,\AA\ for Si(553)-Au -- 10.2\,\AA\ for Si(775)-Au -- , determined from plasmon dispersion is in good agreement with STS data. Clear evidence for coupling between wires is seen beyond nearest neighbor coupling.

Size-Modulation of Plasmonic Nanorings Obtained by the Self-Assembly of Gold Nanoparticles and Block Copolymers

Metal nanoparticles exhibit interesting optical properties due to the collective excitation of conduction electrons called the plasmon. Within appropriate metal nanostructures, cooperative plasmon modes appear and the resonance plasmon frequency is modified. This article reports a simple method for the formation of such structures, in the form of self-assembled nanorings. Rings of alkanethiol-capped gold nanoparticles are obtained by the Langmuir–Blodgett technique and a block copolymer (PS-b-P2VP) template. With this approach, organized nanoparticle arrangements covering a large surface area are obtained. Furthermore, geometric parameters such as ring diameter, ring-to-ring separation, and ring width can be systematically varied by the addition of homopolymer or in situ nanoparticle regrowth. Optical extinction spectra recorded for the nanoparticle rings depend both on ring diameter and particle size. In particular, after in situ particle regrowth, the plasmon extinction spectrum exhibits a red-shift tha...

Plasmon-mediated electron emission from the coronene molecule under fast ion impact

The existence of the collective electronic excitation in polycyclic aromatic hydrocarbon (PAH) molecules has been predicted before on the basis of the presence of a large delocalized $\ensuremath{\pi}$ electron cloud around the carbon skeleton. Here, we present a manifestation of energy and angular distributions of electron emission upon deexcitation of the collective plasmon resonance in coronene, a PAH molecule, under fast ion impact. The angular distributions of these electrons show an unusually enhanced forward-backward angular asymmetry, in contrast to the observed uniform distributions for simpler atomic (Ne) or molecular (${\mathrm{CH}}_{4}$) targets. A simple model of photoelectron angular distribution from an oscillating dipolar plasmon, calculated including the first retardation term in the transition matrix element, provides excellent agreement with the observed distribution. The ratio of forward-to-backward electron emission intensity clearly exhibits a broad peak which is in excellent agreement with the theoretical prediction of the plamson peak. This observation may provide some new inputs towards the astrophysical problem of UV photon absorption by PAHs in the interstellar medium, or in the search for materials suitable for UV plasmonics.

Superconductivity in Potassium-Doped Metallic Polymorphs of MoS2.

Superconducting layered transition metal dichalcogenides (TMDs) stand out among other superconductors due to the tunable nature of the superconducting transition, coexistence with other collective electronic excitations (charge density waves), and strong intrinsic spin-orbit coupling. Molybdenum disulfide (MoS2) is the most studied representative of this family of materials, especially since the recent demonstration of the possibility to tune its critical temperature, Tc, by electric-field doping. However, just one of its polymorphs, band-insulator 2H-MoS2, has so far been explored for its potential to host superconductivity. We have investigated the possibility to induce superconductivity in metallic polytypes, 1T- and 1T'-MoS2, by potassium (K) intercalation. We demonstrate that at doping levels significantly higher than that required to induce superconductivity in 2H-MoS2, both 1T and 1T' phases become superconducting with Tc = 2.8 and 4.6 K, respectively. Unusually, K intercalation in this case is responsible both for the structural and superconducting phase transitions. By adding new members to the family of superconducting TMDs, our findings open the way to further manipulate and enhance the electronic properties of these technologically important materials.

Radiatively Broadened Incandescent Sources

We study the incandescence of a semiconductor system characterized by a radiatively broadened material excitation. We show that the shape of the emission spectrum and the peak emissivity value are determined by the ratio between radiative and nonradiative relaxation rates of the material mode. Our system is a heavily doped quantum well, exhibiting a collective bright electronic excitation in the mid-infrared. The spontaneous emission rate of this collective mode strongly depends on the emission direction and, uncommonly for an intersubband system, can dominate nonradiative scattering processes. Consequently the incandescence spectrum undergoes strong modifications when the detection angle is varied. Incandescence is modeled solving quantum Langevin equations, including a microscopic description of the collective excitations, decaying into electronic and photonic baths. We demonstrate that the emissivity reaches unity value for a well-defined direction and presents an angular radiative pattern that is very...

Superradiant Emission from a Collective Excitation in a Semiconductor.

We report an anomalous wide broadening of the emission spectra of an electronic excitation confined in a two-dimensional potential. We attribute these results to an extremely fast radiative decay rate associated with superradiant emission from the ensemble of confined electrons. Lifetimes extracted from the spectra are below 100 fs and, thus, 6 orders of magnitude faster than for single particle transitions at similar wavelength. Moreover, the spontaneous emission rate increases with the electronic density, as expected for superradiant emission. The data, all taken at 300 K, are in excellent agreement with our theoretical model, which takes into account dipole-dipole Coulomb interaction between electronic excitations. Our experimental results demonstrate that the interaction with infrared light, which is usually considered a weak perturbation, can be a very efficient relaxation mechanism for collective electronic excitations in solids.