The selective optical detection of individual metallic nanoparticles (NPs) with high spatial and temporal resolution is a challenging endeavour, yet is key to the understanding of their optical response and their exploitation in applications from miniaturised optoelectronics and sensors to medical diagnostics and therapeutics. However, only few reports on ultrafast pump-probe spectroscopy on single small metallic NPs are available to date. Here, we demonstrate a novel phase-sensitive four-wave mixing (FWM) microscopy in heterodyne detection to resolve for the first time the ultrafast changes of real and imaginary part of the dielectric function of single small (<40nm) spherical gold NPs. The results are quantitatively described via the transient electron temperature and density in gold considering both intraband and interband transitions at the surface plasmon resonance. This novel microscopy technique enables background-free detection of the complex susceptibility change even in highly scattering environments and can be readily applied to any metal nanostructure.
Theoretical description of oscillations of electron liquid in large metallic nanospheres (with radius of few tens nm) is formulated within random-phase-approximation semiclassical scheme. Spectrum of plasmons is determined including both surface and volume type excitations. It is demonstrated that only surface plasmons of dipole type can be excited by homogeneous dynamical electric field. The Lorentz friction due to irradiation of electro-magnetic wave by plasmon oscillations is analyzed with respect to the sphere dimension. The resulting shift of resonance frequency turns out to be strongly s…
The random-phase-approximation semiclassical scheme for description of plasmon excitations in large metallic nanospheres (with radius 10--100 nm) is developed for a case of presence of dynamical electric field. The spectrum of plasmons in metallic nanosphere is determined including both surface and volume type excitations and their mutual connections. It is demonstrated that only surface plasmons of dipole type can be excited by a homogeneous dynamical electric field. The Lorentz friction due to irradiation of e-m energy by plasmon oscillations is analysed with respect to the sphere dimension.…
The random-phase-approximation semiclassical scheme for description of plasmon excitations in large metallic nanospheres, with radius range 10-60 nm, is formulated in an all-analytical version. The spectrum of plasmons is determined including both surface and volume type excitations and their mutual connections. The various channels for damping of surface plasmons are evaluated and the relevant resonance shifts are compared with the experimental data for metallic nanoparticles of different size located in dielectric medium or on the semiconductor substrate. The strong enhancement of energy tra…
Arrays of metallic nanoparticles support individual and collective plasmonic excitations that contribute to unusual phenomena like surface enhanced Raman scattering, anomalous transparency, negative index, and subwavelength resolution in various metamaterials. We have examined the electromagnetic response of dual Kron's lattice and films containing up to three monolayers of metallic nanospheres. It appears that open cubic Kron's lattice exhibits `soft' electromagnetic response but no negative index behavior. The close-packed arrays behave similarly: there are plasmon resonances and very high t…
With recent experiments investigating the optical properties of progressively smaller plasmonic particles, quantum effects become increasingly more relevant, requiring a microscopic description. Using the density matrix formalism we analyze the photo-excited few-electron dynamics of a small nanosphere. Following the standard derivation of the bulk plasmon we particularly aim on elucidating the role of the Coulomb interaction. Calculating the dielectric susceptibility spectrum in the linear optical response we find discrete resonances resulting from a collective response mediated by the Coulomb…
We show that a dimer made of two gold nanospheres exhibits a remarkable efficiency for second-harmonic generation under femtosecond optical excitation. The detectable nonlinear emission for the given particle size and excitation wavelength arises when the two nanoparticles are as close as possible to contact, as in situ controlled and measured using the tip of an atomic force microscope. The excitation wavelength dependence of the second-harmonic signal supports a coupled plasmon resonance origin with radiation from the dimer gap. This nanometer-size light source might be used for high-resolut…
Assuming that the resonant surface plasmons on a spherical nanoparticle is formed by standing waves of two counter-propagating surface plasmon waves along the surface, by using Mie theory simulation, we find that the dispersions of surface plasmon resonant modes supported by silver nanospheres match that of the surface plasmons on a semi-infinite medium-silver interface very well. This suggests that the resonant surface plasmons of a metal nanosphere can be treated as a propagating surface plasmon wave.
In this work, the plasmon coupling effect between two gold nanospheres on a gold slab is investigated. At plasmon resonance frequencies, electrons on the surface of the slab are absorbed into spheres and contribute to plasmon oscillation. This effect can help enhance the local electric field and optical coupling force between the two spheres.
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…
Collective electron dynamics in plasmonic nanosystems can unfold on timescales in the attosec- ond regime and the direct measurements of plasmonic near-field oscillations is highly desirable. We report on numerical studies on the application of attosecond nanoplasmonic streaking spectroscopy to the measurement of collective electron dynamics in isolated Au nanospheres. The plasmonic field oscillations are induced by a few-cycle NIR driving field and are mapped by the energy of photoemitted electrons using a synchronized, time-delayed attosecond XUV pulse. By a detailed analysis of the amplitud…
A canonical quantization scheme for localized surface plasmons (LSPs) in a metal nanosphere is presented based on a microscopic model composed of electromagnetic fields, oscillators that describe plasmons, and a reservoir that describes excitations other than plasmons. The eigenmodes of this fully quantum electrodynamic theory show a spectrum that includes radiative depolarization and broadening, including redshifting from the quasi-static LSP modes, with increasing particle size. These spectral profiles correctly match those obtained with exact classical electrodynamics (Mie theory). The pres…
We show that interference can be the principle of operation of an all-optical switch and other nanoscale plasmonic interference devices (PIDs). The optical response of two types of planar plasmonic waveguides is studied theoretically: bent chains and Y-shaped configurations of closely-spaced metallic nanospheres. We study symmetric Y-shape arrays as an example of an all-optical switch and demonstrate that effective phase- and amplitude-sensitive control of the output signal can be achieved due to interference effects.
Nanometer-sized metal particles exhibit broadening of the localized surface plasmon resonance (LSPR) in comparison to its value predicted by the classical Mie theory. Using our model for the LSPR dependence on non-local surface screening and size quantization, we quantitatively relate the observed plasmon width to the nanoparticle radius $R$ and the permittivity of the surrounding medium $ε_m$. For Ag nanospheres larger than 8 nm only the non-local dynamical effects occurring at the surface are important and, up to a diameter of 25 nm, dominate over the bulk scattering mechanism. Qualitatively…
The Dicke subradiance and superradiance resulting from the interaction between surface plasmons of a nanosphere and an ensemble of quantum emitters have been investigated using a Green function approach. Based on such an investigation, we propose a scheme for a deterministic multiqubit quantum phase gate. As an example, twoqubit, threequbit, and fourqubit quantum phase gates have been designed and analyzed in detail. Phenomena due to the losses in the metal are discussed. Potential applications of these phenomena to quantuminformation processing are anticipated.
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 …
Progress in ultrafast electron microscopy relies on the development of efficient laser-driven electron sources delivering femtosecond electron pulses to the sample. In particular, recent advances employ photoemission from metal nanotips as coherent point-like femtosecond low-energy electron sources. We report the nonlinear emission of ultrashort electron wave packets from a gold nanotip generated by nonlocal excitation and nanofocusing of surface plasmon polaritons. We verify the nanoscale localization of plasmon-induced electron emission by its electrostatic collimation characteristics. With …
We report on the nanoparticle-size-dependent onset of quantum tunneling of electrons across the sub-nanometer gaps in three different sizes (30, 50, and 80 nm) of highly uniform gold nanosphere dimers. For precision plasmonics, the gap distance is systematically controlled at the level of single C-C bonds via a series of alkanedithiol linkers (C2-C16). The corresponding single-particle scattering spectra reveal that for the larger dimers the onset of quantum effects occurs at larger gap distances: C6 for 80 nm, C5 for 50 nm, and C4 for 30 nm dimers. 2D non-local and quantum-corrected model (QC…
We consider a biased molecular junction subjected to external time-dependent electromagnetic field. The field for two typical junction geometries (bowtie antennas and metal nanospheres) is calculated within finite-difference time-domain technique. Time-dependent transport and optical response of the junctions is calculated within non-equilibrium Green's function approach expressed in a form convenient for description of multi-level systems. We present numerical results for a two-level (HOMO-LUMO) model, and discuss influence of localized surface plasmon polariton modes on transport.
Photoacoustic signal enhancements were observed with a pair of time-delayed femtosecond pulses upon excitation of gold nanosphere colloidal suspension. A systematic experimental investigation of photoacoustic intensity within the delay time, t = 0 to 15 ns, was carried out. The results revealed a significant enhancement factor of ~2 when the pre-pulse energy is 20-30% of the total energy. Pre-pulse and main pulse energy ratios, E(1)p-pol. :E(2)s-pol. were varied to determine the optimal ratio that yields to maximum photoacoustic signal enhancement. This enhancement was ascribed to the initial …
Metallic nano-structures characterised by multiple geometric length scales support low-frequency surface-plasmon modes, which enable strong light localization and field enhancement. We suggest studying such configurations using singular perturbation methods, and demonstrate the efficacy of this approach by considering, in the quasi-static limit, a pair of nearly touching metallic nano-spheres subjected to an incident electromagnetic wave polarized with the electric field along the line of sphere centers. Rather than attempting an exact analytical solution, we construct the pertinent (longitudi…
Optimisation and Precision Tuning of Localised Surface Plasmon Resonance in AuFON Systems
Universidad de Pamplona-Colombia（潘普洛纳大学）；Centro Atómico Bariloche e Instituto Balseiro, Comisión Nacional de Energía Atómica (CNEA) - Universidad Nacional de Cuyo (UNCUYO)（巴里洛切原子中心与巴尔塞罗研究所，国家原子能委员会（CNEA）- 昆卡约国立大学 (UNCUYO)）；Instituto de Nanociencia y Nanotecnología (INN-Bariloche), Consejo Nacional de Investigaciones Científicas y Técnicas (CONICET)（纳米科学与技术研究所（INN-巴里洛切），国家科学研究委员会（CONICET)）
Sub-nanometer 3D morphometric precision of polarisation-resolved wide-field optical extinction microscopy determines the roundness of individual gold nanospheres
Using the ultrafast pump-probe transient absorption spectroscopy, the femtosecond-resolved plasmon-exciton interaction of graphene-Ag nanowire hybrids is experimentally investigated, in the VIS-NIR region. The plasmonic lifetime of Ag nanowire is about 150 femtosecond (fs). For a single layer of graphene, the fast dynamic process at 275 fs is due to the excitation of graphene excitons, and the slow process at 1.4 picosecond (ps) is due to the plasmonic hot electron interaction with phonons of graphene. For the graphene-Ag nanowire hybrids, the time scale of the plasmon-induced hot electron tra…
Fundamental interactions induced by lattice vibrations on ultrafast time scales become increasingly important for modern nanoscience and technology. Experimental access to the physical properties of acoustic phonons in the THz frequency range and over the entire Brillouin zone is crucial for understanding electric and thermal transport in solids and their compounds. Here, we report on the generation and nonlinear propagation of giant (1 percent) acoustic strain pulses in hybrid gold/cobalt bilayer structures probed with ultrafast surface plasmon interferometry. This new technique allows for un…
We report a novel behavior of the surface plasmon linewidth in sodium nanospheres Na$_{1760}$ changing with the electron temperature, which monotonically decreases and bears a discontinuous sudden drop at high electron temperatures. Our calculation is based on the model constructed by splitting the total Hamiltonian of all valence electrons of a metallic nanoparticle into two sub-Hamiltonians and their coupling, and obtained results can be verified by the pump-probe femtosecond spectroscopy experiments. In addition, we propose that it is the size uncertainty of small nanoparticles that yields …
The interaction of chirped femtosecond laser pulses with hybrid materials - materials comprised of plasmon sustaining structures and resonant molecules - is scrutinized using a self-consistent model of coupled Maxwell-Bloch equations. The optical properties of such systems are examined with the example of periodic sinusoidal gratings. It is shown that under strong coupling conditions one can control light transmission using chirped pulses in a spatiotemporal manner. The temporal origin of control relies on chirps non-symmetric in time while the space control is achieved via spatial localizatio…
We study the optical responses of metal nanoparticle chains. Multiple scattering calculations are used to study the extinction cross sections of silver nanosphere chains of finite length embedded in a glass matrix. The transmission and reflection coefficients of periodic 2D arrays of silver nanospheres are also calculated to understand the interaction between nanoparticle chains. The results are in agreement with recent experiments. The splitting of plasmon-resonance modes for different polarizations of the incident light are explored. Results on the effect of disorder are also presented.
The influence of delay-time between two sequential femtosecond pulses on the properties of nanoparticles obtained via laser ablation of gold in ethanol has been studied. The morphological and optical properties of the nanoparticles attained were characterized using high resolution transmission electron microscopy and UV_Vis absorption spectroscopy, respectively. Furthermore, the size distribution of nanoparticles was determined by means of a centrifugal sedimentation particle size analyzer. It is found that the time delay variations lead to corresponding changes in size distribution, plasmon r…
A hot-spot of high local field can be created in between two closely placed metal nanoparticles by irradiating them with an appropriate wavelength and polarization of incident light. The strength of the field at the hot-spot is expected to get enhanced by even up to six orders of magnitude than that of the applied field. Placing a semiconductor quantum dot or an analyte molecule at the hot-spot is an essential step towards harnessing the enhanced field for applications. In this article, we show that it is possible to position a CdTe quantum dot (QD) between two larger silver nanospheres in col…
To combine the advantages of ultrafast femtosecond optics with an on-chip communcation scheme, optical signals with a frequency of several hundreds of THz need to be down-converted to coherent electronic signals of GHz or less. So far, this has not been achieved because of the impedance mismatch within electronic circuits and their overall slow response-time. Here, we demonstrate that 14 fs optical pulses in the near-infrared (NIR) can drive electronic on-chip circuits with a bandwidth up to 10 THz. The corresponding electronic pulses propagate in microscopic striplines on a millimeter scale. …
When in close contact, plasmonic resonances interact and become strongly correlated. In this work we develop a quantum mechanical model, using the language of continuous variables and quantum information, for an array of coupled particle plasmons. This model predicts that when the coupling strength between plasmons approaches or surpasses the local dissipation, a sizable amount of entanglement is stored in the collective modes of the array. We also prove that entanglement manifests itself in far-field images of the plasmonic modes, through the statistics of the quadratures of the field, in wha…
Pan-microbial inactivation technologies that do not require high temperatures, reactive chemical compounds, or UV radiation could address gaps in current infection control strategies and provide efficient sterilization of biologics in the biotechnological industry. Here, we demonstrate that femtosecond (fs) laser irradiation of resonant gold nanoparticles (NPs) under conditions that allow for E-field mediated cavitation and shockwave generation achieve an efficient plasmon-enhanced photonic microbial pathogen inactivation. We demonstrate that this NP-enhanced, physical inactivation approach is…
Recently, asymmetric plasmonic nanojunctions [Karnetzky et. al., Nature Comm. 2471, 9 (2018)] have shown promise as on-chip electronic devices to convert femtosecond optical pulses to current bursts, with a bandwidth of multi-terahertz scale, although yet at low temperatures and pressures. Such nanoscale devices are of great interest for novel ultrafast electronics and opto-electronic applications. Here, we operate the device in air and at room temperature, revealing the mechanisms of photoemission from plasmonic nanojunctions, and the fundamental limitations on the speed of optical-to-electro…
The nonlinear optical dynamics of nano-materials comprised of plasmons interacting with quantum emitters is investigated by a self-consistent model based on the coupled Maxwell-Liouville-von Neumann equations. It is shown that ultra-short resonant laser pulses significantly modify the optical properties of such hybrid systems. It is further demonstrated that the energy transfer between interacting molecules and plasmons occurs on a femtosecond time scale and can be controlled with both material and laser parameters.
Studies of nanoparticle-based optical matter have only considered spherical constituents. Yet nanoparticles with other shapes are expected to have different local electromagnetic field distributions and therefore interactions with neighbors in optical matter arrays. Therefore, one would expect their dynamics to be different as well. We investigate directed-assembly of ordered arrays of plasmonic nanoplatelets in optical line traps demonstrating reconfigurability of the array by altering the phase gradient via holographic beam shaping. The weaker gradient forces on and resultant slower motion o…
We propose a microscopic theory of terahertz (THz) radiation generation on metal gratings under the action of femtosecond laser pulses. In contrast to previous models, only low-frequency currents inside the metal are considered without involving electron emission. The presented model is based on plasmon-enhanced thermal effects and explains the resonant character of optical-to-THz conversion giving an adequate estimation for the full signal energy. Numerical modeling reproduces specific experimental features like delayed character of THz response and low conversion efficiency when the grating …
Electron-hole generation and recombination rates for plasmon emission and absorption in Graphene are presented. The recombination times of carriers due to plasmon emission have been found to be in the tens of femtoseconds to hundreds of picoseconds range. The recombination times depend sensitively on the carrier energy, carrier density, temperature, and the plasmon dispersion. Carriers near the Dirac point are found to have much longer lifetimes compared to carriers at higher energies. Plasmons in a Graphene layer on a polar substrate hybridize with the surface optical phonons and this hybridi…
In magnetoplasmonics, it is possible to tailor the magneto-optical properties of nanostructures by exciting surface plasmon polaritons (SPPs). Thus far, magnetoplasmonic effects have been considered static. Here, we describe ultrafast manifestations of magnetoplasmonics by observing the non-trivial evolution of the transverse magneto-optic Kerr effect within 45-fs pulses reflected from an iron-based magnetoplasmonic crystal. The effect occurs for resonant SPP excitations, displays opposite time derivative signs for different slopes of the resonance, and is explained with the magnetization-depe…
We report the investigation of the generation and detection of GHz coherent acoustic phonons in plasmonic gold nanoparticles superlattices (NPS). The experiments have been performed from an optical femtosecond pump-probe scheme across the optical plasmon resonance of the superlattice. Our experiments allow to estimate the collective elastic response (sound velocity) of the NPS as well as an estimate of the nano-contact elastic stiffness. It appears that the light-induced coherent acoustic phonon pulse has a typical in-depth spatial extension of about 45 nm which is roughly 4 times the optical …
Ultrafast all-optical control of spins with femtosecond laser pulses is one of the hot topics at the crossroads of photonics and magnetism with a direct impact on future magnetic recording. Unveiling light-assisted recording mechanisms for an increase of the bit density beyond the diffraction limit without excessive heating of the recording medium is an open challenge. Here we show that surface plasmon-polaritons in hybrid metal-dielectric structures can provide spatial confinement of the inverse Faraday effect, mediating the excitation of localized coherent spin precession with 0.41 THz frequ…
The interaction between light and metal nanoparticles enables investigations of microscopic phenomena on nanometer length and ultrashort time scales, benefiting from strong confinement and enhancement of the optical field. However, the ultrafast dynamics of these nanoparticles are primarily investigated by multiphoton photoluminescence on picoseconds or photoemission on femtoseconds independently. Here, we presented two-photon photoluminescence (TPPL) measurements on individual Au nanobipyramids (AuNP) to reveal their ultrafast dynamics by two-pulse excitation on a global time scale ranging fr…
