Nonlinearity vs nonlocality with emphasis on bandwidth broadening in semiconductor-based 1d metamaterials.

The physics of nonlinear optical materials is incredibly versatile, with the design of novel materials and structures offering numerous degrees of freedom. Nevertheless, weak inherent nonlinearity of conventional optical materials continues to hinder the progress of a number of important applications. In this study, we delve into the realm of broadband enhancement of nonlinearity within one-dimensional (1d) plasmonic metamaterials, exploring its intricate connection with nonlocality. Specifically, we introduce a phenomenological framework for quantifying the effective third-order nonlinear susceptibility of 1d multiphase plasmonic nanostructures, utilizing heavily doped semiconductors, and subsequently applying this approach using realistic material parameters. Both direct and inverse problems of nonlinearity enhancement have been addressed. Our findings demonstrate a remarkable capability to significantly augment the third-order nonlinear susceptibility across a defined frequency range, while concurrently gauging the impact of nonlocality on this enhancement.

Dramatic Plasmon Response to the Charge-Density-Wave Gap Development in 1T-TiSe_{2}.

1T-TiSe_{2} is one of the most studied charge density wave (CDW) systems, not only because of its peculiar properties related to the CDW transition, but also due to its status as a promising candidate of exciton insulator signaled by the proposed plasmon softening at the CDW wave vector. Using high-resolution electron energy loss spectroscopy, we report a systematic study of the temperature-dependent plasmon behaviors of 1T-TiSe_{2}. We unambiguously resolve the plasmon from phonon modes, revealing the existence of Landau damping to the plasmon at finite momentums, which does not support the plasmon softening picture for exciton condensation. Moreover, we discover that the plasmon lifetime at zero momentum responds dramatically to the band gap evolution associated with the CDW transition. The interband transitions near the Fermi energy in the normal phase are demonstrated to serve as a strong damping channel of plasmons, while such a channel in the CDW phase is suppressed due to the CDW gap opening, which results in the dramatic tunability of the plasmon in semimetals or small-gap semiconductors.

Evidence for a spin acoustic surface plasmon from inelastic atom scattering.

Closed-shell atoms scattered from a metal surface exchange energy and momentum with surface phonons mostly via the interposed surface valence electrons, i.e., via the creation of virtual electron-hole pairs. The latter can then decay into surface phonons via electron-phonon interaction, as well as into acoustic surface plasmons (ASPs). While the first channel is the basis of the current inelastic atom scattering (IAS) surface-phonon spectroscopy, no attempt to observe ASPs with IAS has been made so far. In this study we provide evidence of ASP in Ni(111) with both Ne atom scattering and He atom scattering. While the former measurements confirm and extend so far unexplained data, the latter illustrate the coupling of ASP with phonons inside the surface-projected phonon continuum, leading to a substantial reduction of the ASP velocity and possibly to avoided crossing with the optical surface phonon branches. The analysis is substantiated by a self-consistent calculation of the surface response function to atom collisions and of the first-principle surface-phonon dynamics of Ni(111). It is shown that in Ni(111) ASP originate from the majority-spin Shockley surface state and are therefore collective oscillation of surface electrons with the same spin, i.e. it represents a new kind of collective quasiparticle: a Spin Acoustic Surface Plasmon (SASP).

Real-Time Observation of Phonon-Mediated σ-π Interband Scattering in MgB_{2}.

In systems having an anisotropic electronic structure, such as the layered materials graphite, graphene, and cuprates, impulsive light excitation can coherently stimulate specific bosonic modes, with exotic consequences for the emergent electronic properties. Here we show that the population of E_{2g} phonons in the multiband superconductor MgB_{2} can be selectively enhanced by femtosecond laser pulses, leading to a transient control of the number of carriers in the σ-electronic subsystem. The nonequilibrium evolution of the material optical constants is followed in the spectral region sensitive to both the a- and c-axis plasma frequencies and modeled theoretically, revealing the details of the σ-π interband scattering mechanism in MgB_{2}.

Odd-frequency superconductivity induced in topological insulators with and without hexagonal warping.

We study the effect of the Fermi surface anisotropy on the odd-frequency spin-triplet pairing component of the induced pair potential. We consider a superconductor/ ferromagnetic insulator (S/FI) hybrid structure formed on the 3D topological insulator (TI) surface. In this case three ingredients ensure the possibility of the odd-frequency pairing: (1) the topological surface states, (2) the induced pair potential, and (3) the magnetic moment of a nearby ferromagnetic insulator. We take into account the strong anisotropy of the Dirac point in topological insulators when the chemical potential lies well above the Dirac cone and its constant energy contour has a snowflake shape. Within this model, we propose that the S/FI boundary should be properly aligned with respect to the snowflake constant energy contour to have an odd-frequency symmetry of the corresponding pairing component and to insure the Majorana bound state at the S/FI boundary. For arbitrary orientation of the boundary, the Majorana bound state is absent. This provides a selection rule to the realization of Majorana modes in S/FI hybrid structures, formed on the topological insulator surface.

On the stability of the electronic system in transition metal dichalcogenides.

Based on first-principles calculations, we prove that the origin of charge-density wave formation in metallic layered transition metal dichalcogenides (TMDC) is not due to an electronic effect, like the Fermi surface (FS) nesting, as it had been proposed. In particular, we consider NbSe2, NbS2, TaSe2, and TaS2 as representative examples of 2H-TMDC polytypes. Our main result consists that explicit inclusion of the matrix elements in first-principles calculations of the electron susceptibility [Formula: see text] removes, due to strong momentum dependence of the matrix elements, almost all the information about the FS topologies in the resulting [Formula: see text]. This finding strongly supports an interpretation in which the momentum dependence of the electron-phonon interaction is the only reason why the phenomenon of charge-density waves appears in this class of materials.

Interplay of Surface and Dirac Plasmons in Topological Insulators: The Case of Bi_{2}Se_{3}.

We have investigated plasmonic excitations at the surface of Bi_{2}Se_{3}(0001) via high-resolution electron energy loss spectroscopy. For low parallel momentum transfer q_{∥}, the loss spectrum shows a distinctive feature peaked at 104 meV. This mode varies weakly with q_{∥}. The behavior of its intensity as a function of primary energy and scattering angle indicates that it is a surface plasmon. At larger momenta (q_{∥}~0.04 Å^{-1}), an additional peak, attributed to the Dirac plasmon, becomes clearly defined in the loss spectrum. Momentum-resolved loss spectra provide evidence of the mutual interaction between the surface plasmon and the Dirac plasmon of Bi_{2}Se_{3}. The proposed theoretical model accounting for the coexistence of three-dimensional doping electrons and two-dimensional Dirac fermions accurately represents the experimental observations. The results reveal novel routes for engineering plasmonic devices based on topological insulators.

Low-energy dielectric screening in Pd and PdHx systems.

Modifications in dielectric properties of palladium upon absorption of hydrogen are investigated theoretically in the low-energy (0-2 eV) region. The calculations were performed with full inclusion of the electronic band structure obtained within a self-consistent pseudopotential approach. In particular, we trace the evolution of the acoustic-like plasmon (AP) found previously in clean Pd with increasing hydrogen concentration. It exists in PdHx up to the hydrogen content x corresponding to the complete filling of the 4d Pd-derived energy bands because of the presence of two kinds of carriers at the Fermi surface. At higher H concentration the AP disappears since only one kind of carrier within the sp-like energy band exists at the Fermi level. Additionally, we investigate the spatial distribution inside the crystal of a potential caused by a time-dependent external perturbation and observe drastic modifications in the screening properties in the PdHx systems with energy and with hydrogen concentration.

Anisotropic dispersion and partial localization of acoustic surface plasmons on an atomically stepped surface: Au(788).

Understanding acoustic surface plasmons (ASPs) in the presence of nanosized gratings is necessary for the development of future devices that couple light with ASPs. We show here by experiment and theory that two ASPs exist on Au(788), a vicinal surface with an ordered array of monoatomic steps. The ASPs propagate across the steps as long as their wavelength exceeds the terrace width, thereafter becoming localized. Our investigation identifies, for the first time, ASPs coupled with intersubband transitions involving multiple surface-state subbands.

Correlated motion of electrons on the Au(111) surface: anomalous acoustic surface-plasmon dispersion and single-particle excitations.

The linear dispersion of the low-dimensional acoustic surface plasmon (ASP) opens perspectives in energy conversion, transport, and confinement far below optical frequencies. Although the ASP exists in a wide class of materials, ranging from metal surfaces and ultrathin films to graphene and topological insulators, its properties are still largely unexplored. Taking Au(111) as a model system, our combined experimental and theoretical study revealed an intriguing interplay between collective and single particle excitations, causing the ASP associated with the Shockley surface state to be embedded within the intraband transitions without losing its sharp character and linear dispersion.

Tuning the plasmon energy of palladium-hydrogen systems by varying the hydrogen concentration.

First-principles calculations are performed to obtain the dielectric function and loss spectra of bulk PdH(x). Hydrogen concentrations between x = 0 and 1 are considered. The calculated spectra are dominated by a broad peak that redshifts in energy with x. The obtained bulk dielectric function is employed to compute the loss spectra of PdH(x) spherical nanoparticles as a function of x. The dominant plasmon peak in the spherical nanoparticle is lowered in energy with respect to the bulk case. However, the dependence of the resonance energy on the hydrogen concentration is roughly similar to that in bulk.

Multiscale Theoretical Modeling of Plasmonic Sensing of Hydrogen Uptake in Palladium Nanodisks.

We study theoretically the optical properties of palladium nanodisks during hydrogen uptake. A combination of an ab initio quantum mechanical description of the Pd-H dielectric properties and a full electrodynamical study of light scattering in the H-modified Pd nanodisks allows us to trace the shift of the localized surface plasmon as a function of the H concentration in the Pd-H disk. We follow the evolution of the plasmon peak energy for different admixtures of the Pd-H α and ß phases and interpret quantitatively the experimental sensitivity of the plasmon energy shift to the structural inhomogeneity upon H absorption. Our multiscale theoretical framework provides a solid background for plasmonic sensing of structural domains, as well as for identifying H saturation conditions in metal hydride systems.

Time-dependent electron phenomena at surfaces.

Femtosecond and subfemtosecond time scales typically rule electron dynamics at metal surfaces. Recent advance in experimental techniques permits now remarkable precision in the description of these processes. In particular, shorter time scales, smaller system sizes, and spin-dependent effects are current targets of interest. In this article, we use state-of-the-art theoretical methods to analyze these refined features of electron dynamics. We show that the screening of localized charges at metal surfaces is created locally in the attosecond time scale, while collective excitations transfer the perturbation to larger distances in longer time scales. We predict that the elastic width of the resonance in excited alkali adsorbates on ferromagnetic surfaces can depend on spin orientation in a counterintuitive way. Finally, we quantitatively evaluate the electron-electron and electron-phonon contributions to the electronic excited states widths in ultrathin metal layers. We conclude that confinement and spin effects are key factors in the behavior of electron dynamics at metal surfaces.

Potential energy landscape for hot electrons in periodically nanostructured graphene.

We explore the spatial variations of the unoccupied electronic states of graphene epitaxially grown on Ru(0001) and observed three unexpected features: the first graphene image state is split in energy; unlike all other image states, the split state does not follow the local work function modulation, and a new interfacial state at +3 eV appears on some areas of the surface. First-principles calculations explain the observations and permit us to conclude that the system behaves as a self-organized periodic array of quantum dots.

Time-dependent screening of a point charge at a metal surface.

The space-time evolution of the dynamical screening charge density caused by a suddenly created point charge at the Cu(111) surface is investigated in the linear response approximation. Considering a thin slab as a model for the Cu(111) surface, we investigate the confinement effects on dynamical screening as well. The results have been obtained on the basis of self-consistent evaluation of the energy-momentum-dependent response function, taking into account the realistic surface band structure of Cu(111). At the initial stage, we observe fast long-range charge density oscillations due to excitation of the surface plasmon modes. Then we observe the propagation of the shock wave of the electron-hole excitations along the slab with velocity determined by the Fermi velocity of bulk Cu. At longer times, we have identified the propagation along the two slab surfaces of a much slower (with velocity ∼ 0.3 au, close to the Fermi velocity of the Cu(111) surface state) charge disturbance due to acoustic surface plasmon. The role of the energy band gap in the direction perpendicular to the surface in establishing the screening is also addressed.

Pi resonance of chemisorbed alkali atoms on noble metals.

We have performed a joint experimental and theoretical study of the unoccupied electronic structure of alkali adsorbates on the (111) surfaces of Cu and Ag. Combining angle- and time-resolved two-photon photoemission spectroscopy with wave packet propagation calculations we show that, along with the well known sigma resonance oriented along the surface normal, there exist long-lived alkali-localized resonances oriented parallel to the surface (pi symmetry). These new resonances are stabilized by the projected band gap of the substrate and emerge primarily from the mixing of the p and d Rydberg orbitals of the free alkali atom modified by the interaction with the surface.

Extreme ultrafast dynamics of quasiparticles excited in surface electronic bands.

We develop a many-body description of the nonadiabatic dynamics of quasiparticles in surface bands valid on an extremely ultrashort time scale by combining the formalism for the calculation of quasiparticle survival probabilities with the self-consistent treatment of the electronic response of the system. Applying this approach to the benchmark Cu(111) surface, we assess the behavior and intervals of preasymptotic electron and hole dynamics in surface bands and locate the transition to the asymptotic regime of the exponential quasiparticle decay characterized by the corrected Fermi golden rule-type of transition rate. The general validity of these findings enables distinguishing the various regimes of ultrafast electron dynamics that may be revealed in time resolved experiments.

Role of elastic scattering in electron dynamics at ordered alkali overlayers on Cu(111).

Scanning tunneling spectroscopy of p(2 x 2) Cs and Na ordered overlayers on Cu(111) reveals similar line widths of quasi-two-dimensional quantum well states despite largely different binding energies. Detailed calculations show that 50% of the line widths are due to electron-phonon scattering while inelastic electron-electron scattering is negligible. The mechanism of enhanced elastic scattering due to Brillouin zone backfolding contributes the remaining width.

Band structure versus dynamical exchange-correlation effects in surface plasmon energy and damping: a first-principles calculation.

A first-principles parameter-free calculation that includes full three-dimensional band structure and dynamical exchange correlations is reported for the dynamical surface response and surface plasmon (SP) on a simple metal prototype surface Mg(0001). We demonstrate that band structure effects have a more profound impact on the SP characteristics than dynamical exchange correlations. A comparison with jellium and one-dimensional potential evaluations shows that the band structure is of paramount importance for the correct description of the SP linewidth and also leads to a better description of the SP energy dispersion. The inclusion of the exchange-correlation kernel results in a better agreement with experimental data. We show that lateral crystal local field effects have a negligible impact on the SP properties. Significant anisotropy is predicted for the SP linewidth.