Hybrid plasmonic photonic structures combine the plasmonic response with the photonic band gap, holding promise for utilization as optical switches and sensors. Here, we demonstrate the active modulation of the optical response in such structures with two different external stimuli, e.g. laser pulses and bacteria. First, we report the fabrication of a miniaturized (5 x 5 mm) indium tin oxide (ITO) grating employing femtosecond laser micromachining, and we show the possibility to modulate the photonic band gap in the visible via ultrafast photoexcitation in the infrared part of the spectrum. Note that the demonstrated time response in the picosecond range of the spectral modulation have an industrial relevance. Moreover, we manufacture one-dimensional photonic crystals consisting of a solution-processed dielectric Bragg stack exposing a top-layer of bio-active silver. We assign the bacterial responsivity of the system to polarization charges at the Ag/bacterium interface, giving rise to an overall blue shift of the photonic band gap.
We demonstrate that ultrafast carrier excitation can drastically affect electronic structures and induce brief surface plasmonic response in non-plasmonic metals, potentially creating a plasmonic switch. Using first-principles molecular dynamics and Kubo-Greenwood formalism for laser-excited tungsten we show that carrier heating mobilizes d electrons into collective inter and intraband transitions leading to a sign flip in the imaginary optical conductivity, activating plasmonic properties for the initial non-plasmonic phase. The drive for the optical evolution can be visualized as an increasi…
Efficient frequency conversion techniques are crucial to the development of plasmonic metasurfaces for information processing and signal modulation. In principle, nanoscale electric-field confinement in nonlinear materials enables higher harmonic conversion efficiencies per unit volume than those attainable in bulk materials. Here we demonstrate efficient second-harmonic generation (SHG) in a serrated nanogap plasmonic geometry that generates steep electric field gradients on a dielectric metasurface. An ultrafast pump is used to control plasmon-induced electric fields in a thin-film material …
Coherent broadband excitation of plasmons brings ultrafast photonics to the nanoscale. However, to fully leverage this potential for ultrafast nanophotonic applications, the capacity to engineer and control the ultrafast response of a plasmonic system at will is crucial. Here, we develop a framework for systematic control and measurement of ultrafast dynamics of near-field hotspots. We show deterministic design of the coherent response of plasmonic antennas at femtosecond timescales. Exploiting the emerging properties of coupled antenna configurations, we use the calibrated antennas to enginee…
Excitation of coherent optical phonons in solids provides a pathway for ultrafast modulation of light on a sub-ps timescale. Here, we report on efficient 3.6 THz modulation of light reflected from hybrid metal/semiconductor plasmonic crystals caused by lattice vibrations in a few nm thick layer of elemental tellurium. We observe that surface plasmon polaritons contribute significantly to photoinduced formation of this thin layer at the interface between a telluride-based II-VI semiconductor, such as (Cd,Mg)Te or (Cd,Mn)Te, and a one-dimensional gold grating. The change in interface composition…
We report that femtosecond surface plasmon polariton pulses can propagate along a metal-dielectric waveguide and that they can be modulated on the femtosecond timescale by direct ultrafast optical excitation of the metal, thereby offering unprecedented terahertz plasmonic bandwidth - a key missing component in the development of surface plasmons as information carriers for next generation nanophotonic devices.
We demonstrate that the dispersion of surface plasmon polaritons in a periodically perforated gold film can be efficiently manipulated by femtosecond laser pulses with the wavelengths far from the intrinsic resonances of gold. Using a time- and frequency- resolved pump-probe technique we observe shifting of the plasmon polariton resonances with response times from 200 to 800 fs depending on the probe photon energy, through which we obtain comprehensive insight into the electron dynamics in gold. We show that Wood anomalies in the optical spectra provide pronounced resonances in differential tr…
We report a measurement on the temporal response of a plasmonic antenna at the femtosecond time scale. The antenna consists of a square array of nanometer-size gold rods. We find that the far-field dispersion of light reflected from the plasmonic antenna is less than that of a 1.2 mm thick glass slide. Assuming a simple oscillating dipole model this implies that the near-field of the antenna may be used as an electron switch that responds faster than 20 fs. Alternatively, ultrafast electron diffraction may be used to investigate the near-field dynamics of the plasmonic antenna.
Surface plasmon polaritons (SPP or SP) are electromagnetic waves propagating along metal dielectric interfaces and existing over a wide range of frequencies. They have become popular because of their sub-wavelength confinement and the possibility to perform ultrasensitive optical measurements. Driven by tremendous progress in nanofabrication techniques and ultrafast laser technologies the applications of SP nanooptics extend beyond the border of nanoplasmonics. Here we review how using novel hybrid multilayer structures combining different functionalities allows to develop active plasmonic dev…
The excitation of plasmonic nanoparticles by ultrashort laser pulses sets in motion a complex ultrafast relaxation process involving the gradual re-equilibration of the system's electron gas, lattice and environment. One of the major hurdles in studying these processes is the lack of direct measurements of the dynamic temperature evolution of the system subcomponents. We measured the dynamic optical response of ensembles of plasmonic Au nanoparticles following ultrashort-pulse excitation and we compared it with the corresponding static optical response as a function of the increasing temperatu…
The theory of energy transfer dynamics of a pair of donor and acceptor molecules located in the plasmonic hot spots is developed by means of the master equation approach and the electromagnetic Green's tensor technique. A nonlocal effect has been considered by using a hydrodynamic model. The coherent interaction between the two molecules in plasmonic nanostructures is investigated under some strong coupling conditions. It is shown that the energy transfer efficiency of a pair of molecules can be improved largely and the transfer time decreases to dozens of femtoseconds when the contribution of…
Spasers have been theoretically predicted and experimentally observed and promise to deliver new exciting nanophotonic and biomedical applications. Here we theoretically investigate ultrafast dynamical properties of spasers with external plasmonic feedback. We consider a spaser both as a nanoscale source and detector of plasmons which could be used to design novel nano-imaging and sensing techniques. We show that, as with conventional lasers, spasers are sensitive to external feedback. However, unlike the lasers, spasers have faster relaxation dynamics which could be used to develop new ultras…
We explore the nonlinear response of plasmonic materials driven by ultrashort pulses of electromagnetic radiation with temporal duration of few femtoseconds and high peak intensity. By developing the Fokker-Planck-Landau theory of electron collisions, we solve analytically the collisional integral and derive a novel set of hydrodynamical equations accounting for plasma dynamics at ultrashort time scales. While in the limit of small light intensities we recover the well established Drude model of plasmas, in the high intensity limit we observe nonlinear quenching of collision-induced damping le…
Femtosecond-scale polarization state conversion is experimentally found in optical response of a plasmonic nanograting by means of time-resolved polarimetry. Simultaneous measurements of the Stokes parameters as a function of time with an averaging time-gate of 130 fs reveal a remarkable alteration of polarization state inside a single fs-pulse reflected from a plasmonic crystal. Time-dependent depolarization is experimentally found and described within an analytical model which predicts the four-fold enhancement of the polarization conversion effect with the use of the narrower gate. The effe…
Nowadays, via controlling surface plasmons (SPs) on elaborate man-made structures, plasmonics aiming at manipulating light beyond the diffraction limit has aroused great interest. Here, nevertheless, we demonstrate in short-pulse laser ablation ultrafast active plasmonic structures spontaneously generate in virtue of plasmonic effects rather than human ingenuity. First, the splitting of laser-induced subwavelength gratings that is experimentally evidenced on ZnO, Si, and GaAs, is confirmed to originate in the conversion of SP modes from the resonant to the nonresonant mode and further to the i…
Topological photonics has revolutionized our understanding of light propagation, but most of current studies are focused on designing a static photonic structure. Developing a dynamic photonic topological platform to switch multiple topological functionalities at ultrafast speed is still a great challenge. Here we demonstrate an ultrafast reprogrammable plasmonic topological insulator, where the topological propagation route can be dynamically steered at nanosecond-level switching time, namely more than 10^7 times faster than the current state-of-the-art. This orders-of-magnitude improvement i…
Ultrafast nanophotonics is an emerging research field aimed at the development of nanodevices capable of light modulation with unprecedented speed. A promising approach exploits the optical nonlinearity of nanostructured materials (either metallic or dielectric) to modulate their effective permittivity via interaction with intense ultrashort laser pulses. While the ultrafast temporal dynamics of such nanostructures following photoexcitation has been studied in depth, sub-ps transient spatial inhomogeneities taking place at the nanoscale have been so far almost ignored. Here we theoretically pr…
Simultaneous spatio-temporal confinement of energetic electron pulses to femtosecond and nanometer scales is a topic of great interest in the scientific community, given the potential impact of such development on a wide spectrum of scientific and industrial applications. For example, in ultrafast electron scattering, nanoscale probes would enable accurate maps of structural dynamics in materials with nanoscale heterogeneity, thereby understanding the role of boundaries and defects on macroscopic properties. On the other hand, advances in this field are mostly limited by the electron source br…
All-optical switches have attracted attention because they can potentially overcome the speed limitation of electric switches. However, ultrafast, energy-efficient all-optical switches have been challenging to realize due to the intrinsically small optical nonlinearity in existing materials. As a solution, we propose graphene-loaded deep-subwavelength plasmonic waveguides (30 nm x 20 nm). Thanks to extreme light confinement, we have significantly enhanced optical nonlinear absorption in graphene, and achieved ultrafast all-optical switching with a switching energy of 35 fJ and a switching time…
Ultrafast lasers generating high repetition rate ultrashort pulses through various mode-locking methods can benefit many important applications including communication, materials processing, astronomical observation, etc. For decades, mode-locking based on dissipative four-wave-mixing (DFWM) has been fundamental in producing pulses with repetition rates on the order of gigahertz (GHz), where multiwavelength comb filters and long nonlinear components are elemental. Recently, this method has been improved using filter-driven DFWM, which exploits both the filtering and nonlinear features of silic…
We investigate the ultrafast nonlinear dynamics of light emitted in an active plasmonic waveguide composed of a thin film of gold sandwiched by two silicon layers immersed in externally pumped Al$_2$O$_3$:Er$^{3+}$. We model optical propagation in such a dissipative system through a generalized cubic Ginzburg-Landau equation accounting for the amplification of the active medium and the effect of absorption and thermo-modulational nonlinearity of gold. We find that heating heavily affects the propagation of temporal dissipative solitons in such a plasmonic waveguide by producing a soliton self-…
Spatio-temporal control of ultrafast plasmon resonances has gained research interest in recent years because of their tremendous implications in nonlinear optics and ultrafast quantum technology. In particular, the lifetime of ultrashort plasmon oscillations has become a debatable subject in recent experimental and theoretical studies to fulfill the future challenges concerning their effective employment in the vast applications of the plasmonic industry. Here, we examined the temporal properties of nonlinear plasmonic modes in metal nanostructures by interacting them with quantum objects in t…
Ultrafast pump-probe measurements of plasmonic nanostructures probe the non-equilibrium behavior of excited carriers, which involves several competing effects obscured in typical empirical analyses. Here we present pump-probe measurements of plasmonic nanoparticles along with a complete theoretical description based on first-principles calculations of carrier dynamics and optical response, free of any fitting parameters. We account for detailed electronic-structure effects in the density of states, excited carrier distributions, electron-phonon coupling, and dielectric functions which allow us…
Vortex-carrying matter waves, such as chiral electron beams, are of significant interest in both applied and fundamental science. Continuous wave electron vortex beams are commonly prepared via passive phase masks imprinting a transverse phase modulation on the electron's wave function. Here, we show that femtosecond chiral plasmonic near fields enable the generation and dynamic control on the ultrafast timescale of an electron vortex beam. The vortex structure of the resulting electron wavepacket is probed in both real and reciprocal space using ultrafast transmission electron microscopy. Thi…
We consider light scattering by a coated magneto-plasmonic nanoparticle (MPNP) with a Kerr-type nonlinear plasmonic shell and a magneto-optic core. Such structure features two plasmon dipole modes, associated with electronic oscillations on the inner and outer surfaces of the shell. Driven in a nonlinear regime, each mode exhibits a bistable response. Bistability of an inner plasmon leads to switching between this state and a Fano resonance (Fano switching). Once the external light intensity exceeds the critical value, the bistability zones of both eigen modes overlap yielding optical tristabi…
Starting from first principles, we theoretically model the nonlinear temporal dynamics of gold-based plasmonic devices resulting from the heating of their metallic components. At optical frequencies, the gold susceptibility is determined by the interband transitions around the X,L points in the first Brillouin zone and thermo-modulational effects ensue from Fermi smearing of the electronic energy distribution in the conduction band. As a consequence of light-induced heating of the conduction electrons, the optical susceptibility becomes nonlinear. In this paper we describe, for the first time …
We predict a dynamic metallization effect where an ultrafast (single-cycle) optical pulse with a field less or on the order of 1 V/Angstrom causes plasmonic metal-like behavior of a dielectric film with a few-nm thickness. This manifests itself in plasmonic oscillations of polarization and a significant population of the conduction band evolving on a femtosecond time scale. These phenomena are due a combination of both adiabatic (reversible) and diabatic (for practical purposes irreversible) pathways.
The strong-field control of plasmonic nanosystems opens up new perspectives for nonlinear plasmonic spectroscopy and petahertz electronics. Questions, however, remain regarding the nature of nonlinear light-matter interactions at sub-wavelength spatial and ultrafast temporal scales. Addressing this challenge, we investigated the strong-field control of the plasmonic response of Au nanoshells with a SiO$_2$ core to an intense laser pulse. We show that the photoelectron energy spectrum from these core-shell nanoparticles displays a striking transition between the weak and strong-field regime. Th…
Metafibers expand the functionalities of conventional optical fibers to unprecedented nanoscale light manipulations by integrating metasurfaces on the fiber tips, becoming an emerging light-coupling platform for both nanoscience and fiber optics communities. Mostly exploring the isolated bare fibers, current metafibers remain as proof-of-concept demonstrations due to a lack of standard interfaces with the universal fiber networks. Here, we develop new methodologies to fabricate well-defined plasmonic metasurfaces directly on the end facets of commercial single mode fiber jumpers using standard…
The research area of plasmonics promises devices with ultrasmall footprint operating at ultrafast speeds and with lower energy consumption compared to conventional electronics. These devices will operate with light and bridge the gap between microscale dielectric photonic systems and nanoscale electronics. Recent research advancements in nanotechnology and optics have led to the creation of a plethora of new plasmonic designs. Among the most promising are nanoscale antennas operating at optical frequencies, called nanoantennas. Plasmonic nanoantennas can provide enhanced and controllable light…
Ultrafast laser measurements probe the non-equilibrium dynamics of excited electrons in metals with increasing temporal resolution. Electronic structure calculations can provide a detailed microscopic understanding of hot electron dynamics, but a parameter-free description of pump-probe measurements has not yet been possible, despite intensive research, because of the phenomenological treatment of electron-phonon interactions. We present ab initio predictions of the electron-temperature dependent heat capacities and electron-phonon coupling coefficients of plasmonic metals. We find substantial…
We predict a new type of ultrafast third-order nonlinearity of surface plasmon polaritons (SPP) in planar magneto-plasmonic structures caused by the inverse Faraday effect (IFE). Planar SPPs with a significant longitudinal component of the electric field act via the IFE as an effective transverse magnetic field. Its response to the plasmon propagation leads to strong ultrafast self-action which manifests itself through a third-order nonlinearity. We derive a general formula and analytical expressions for the IFE-related nonlinear susceptibility for two specific planar magneto-plasmonic structu…
Photonic crystals can integrate plasmonic materials such as indium tin oxide (ITO) in their structure. Exploiting ITO plasmonic properties it is possible to tune the photonic band gap of the photonic crystal upon the application of an external stimuli. In this work, we have fabricated a one-dimensional multilayer photonic crystal via radiofrequency sputtering and we have triggered its optical response with ultrafast pump-probe spectroscopy. Upon photoexcitation we observe a change in the refractive index of indium tin oxide. Such effect has been used to create a photonic crystal that change it…
Plasmonic metasurfaces based on the extraordinary optical transmission effect (EOT) can be designed to efficiently transmit specific spectral bands from the visible to the far-infrared regimes, offering numerous applications in im-portant technological fields such as compact multispectral imaging, biological and chemical sensing, or color displays. However, due to their subwavelength nature, EOT metasurfaces are nowadays fabricated with nano- and micro-lithographic techniques, requiring many processing steps and carried out in expensive cleanroom environments. In this work, we propose and expe…
We study theoretically the cascaded four-wave mixing (FWM) in broadband tapered plasmonic nanoantennas and demonstrate a 300-fold increase in nonlinear frequency conversion detected in the main lobe of the nanoantenna far-field pattern. This is achieved by tuning the elements of the nanoantenna to resonate frequencies involved into the FWM interaction. Our findings have a potentially broad application in ultrafast nonlinear spectroscopy, sensing, on-chip optical frequency conversion, nonlinear optical metamaterials and photon sources.
Plasmonic waveguides provide an integrated platform to develop efficient nanoscale ultrafast photonic devices. Theoretical models that describe nonlinear optical phenomena in plasmonic waveguides, usually, only incorporate bulk nonlinearities, while nonlinearities that arise from metallic constituents remained unexplored. In this work, we present a method that enables a generalized treatment of the nonlinearities present in plasmonic waveguides and use it to calculate second-harmonic generation from free electrons through a hydrodynamic nonlocal description. As a general application of our met…
Watching the motion of electrons on their natural nanometre length- and femtosecond time scales is a fundamental goal and an open challenge of contemporary ultrafast science. Optical techniques and electron microscopy currently mostly provide either ultrahigh temporal or spatial resolution, yet, microscopy techniques with combined space-time resolution need further development. Here we create an ultrafast electron source by plasmon nanofocusing on a sharp gold taper and implement this source in an ultrafast point-projection electron microscope. This source is used, in an optical pump - electro…
Epsilon-near-zero (ENZ) materials have shown significant potential for nonlinear optical applications due to their ultrafast hot carriers and consequent optical nonlinearity enhancement. Modified poly(3,4-ethylenedioxythiophene) (PEDOT) films show metallic characteristics and a resultant ENZ wavelength near 1550nm through polar solvent treatment and annealing. The metallic PEDOT film exhibits an intrinsic optical nonlinear response that is comparable to gold and 100-fold higher than typical inorganic semiconductor ENZ materials due to π-conjugated delocalized electrons. Hot carriers generate a…
Using long-range surface plasmon polaritons light can propagate in metal nano-scale waveguides for ultracompact opto-electronic devices. Gold is an important material for plasmonic waveguides, but although its linear optical properties are fairly well understood, the nonlinear response is still under investigation. We consider propagation of pulses in ultrathin gold strip waveguides, modeled by the nonlinear Schrödinger equation. The nonlinear response of gold is accounted for by the two-temperature model, revealing it as a delayed nonlinearity intrinsic in gold. The consequence is that the me…
The inverse Faraday effect is a magneto-optical process allowing the magnetization of matter by an optical excitation carrying a non-zero spin or orbital moment of light. This phenomenon was considered until now as symmetric; right or left circular polarizations generate magnetic fields oriented in the direction of light propagation or in the counter-propagating direction. Here, we demonstrate that by manipulating the spin density of light in a plasmonic nanostructure, we generate a chiral inverse Faraday effect, creating a strong magnetic field of 500 mT only for one helicity of the light, th…
