Self-assembly processes allow us to design and create complex nanostructures using molecules as building blocks and surfaces as scaffolds. This autonomous driven construction is possible due to a complex thermodynamic balance of molecule-surface interactions. As such, nanoscale guidance and control over this process is hard to achieve. Here we use the highly localized light-to-chemical-energy conversion of plasmonic materials to spatially cleave Au-S bonds on pre-determined locations within a single nanoparticle, enabling unprecedented control over this archetypal system for molecular self-assembly. Our method offers nanoscale precision and high-throughput light-induced tailoring of the surface chemistry of individual and packed nano-sized metallic structures by simply varying wavelength and polarization of the incident light. Assisted by single-molecule super-resolution fluorescence microscopy, we image, quantify and shed light onto the plasmon-induced desorption mechanism. We show that plasmon-induced photo-desorption enables sub-diffraction multiplexing, selective positioning of nanomaterials and even sorting and purification of colloidal nanoparticles.
Pump-probe spectroscopy is central for exploring ultrafast dynamics of fundamental excitations, collective modes and energy transfer processes. Typically carried out using conventional diffraction-limited optics, pump-probe experiments inherently average over local chemical, compositional, and electronic inhomogeneities. Here we circumvent this deficiency and introduce pump-probe infrared spectroscopy with ~20 nm spatial resolution, far below the diffraction limit, which is accomplished using a scattering scanning near-field optical microscope (s-SNOM). This technique allows us to investigate …
Electrically-driven optical antennas can serve as compact sources of electromagnetic radiation operating at optical frequencies. In the most widely explored configurations, the radiation is generated by electrons tunneling between metallic parts of the structure when a bias voltage is applied across the tunneling gap. Rather than relying on an inherently inefficient inelastic light emission in the gap, we suggest to use a ballistic nanoconstriction as the feed element of an optical antenna supporting plasmonic modes. We discuss the underlying mechanisms responsible for the optical emission, an…
Nanoscale localization of electromagnetic fields near metallic nanostructures underpins the fundamentals and applications of plasmonics. The unavoidable energy loss from plasmon decay, initially seen as a detriment, has now expanded the scope of plasmonic applications to exploit the generated hot carriers. However, quantitative understanding of the spatial localization of these hot carriers, akin to electromagnetic near-field maps, has been elusive. Here we spatially map hot-electron-driven reduction chemistry with 15 nanometre resolution as a function of time and electromagnetic field polariz…
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…
Nanophotonic (nanoplasmonic) structures confine, guide, and concentrate light on the nanoscale. Advancement of nanophotonics critically depends on active nanoscale control of these phenomena. Localized control of the insulator and metallic phases of vanadium dioxide (VO2) would open up a universe of applications in nanophotonics via modulation of the local dielectric environment of nanophotonic structures allowing them to function as active devices. Here we show dynamic reversible control of VO2 insulator-to-metal transition (IMT) locally on the scale of 15 nm or less and control of nanoantenn…
We theoretically explore the notion of nonreciprocal near-zone manipulation of electromagnetic fields within subwavelength plasmonic nanostructures embedded in magneto-optical materials. We derive an analytical model predicting a strong, magneto-optically induced time-reversal symmetry breaking of localized plasmonic resonances in topologically symmetric structures. Our numerical simulations of plasmon excitations reveal a considerable near-zone power flow rotation within such hybrid nanostructures, demonstrating nanoscale nonreciprocity. This can be considered as another mechanism for tuning …
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…
All-optical switching (AOS) of magnetic domains by femtosecond laser pulses was first observed in the transition metal-rare earth (TM-RE) alloy GdFeCo1-5; this phenomenon demonstrated the potential for optical control of magnetism for the development of ever faster future magnetic recording technologies. The technological potential of AOS has recently increased due to the discovery of the same effect in other materials, including RE-free magnetic multilayers6,7. However, to be technologically meaningful, AOS must compete with the bit densities of conventional storage devices, restricting optic…
We explore nanoscale hydrodynamical effects on synthesis and self-assembly of cadmium sulfide nanotubes oriented along one direction. These nanotubes are synthesized by horizontal capillary flow of two different chemical reagents from opposite directions through nanochannels of porous anodic alumina which are used primarily as nanoreactors. We show that uneven flow of different chemical precursors is responsible for directionally asymmetric growth of these nanotubes. On the basis of structural observations using scanning electron microscopy, we argue that chemohydrodynamic convective interfaci…
Boosting nonlinear frequency conversion in extremely confined volumes remains a key challenge in nano-optics, nanomedicine, photocatalysis, and background-free biosensing. To this aim, field enhancements in plasmonic nanostructures are often exploited to effectively compensate for the lack of phase-matching at the nanoscale. Second harmonic generation (SHG) is, however, strongly quenched by the high degree of symmetry in plasmonic materials at the atomic scale and in nanoantenna designs. Here, we devise a plasmonic nanoantenna lacking axial symmetry, which exhibits spatial and frequency mode o…
The plasmon modes of pristine and impurity doped graphene are calculated, using a real-space theory which determines the non-local dielectric response within the random phase approximation. A full diagonalization of the polarization operator is performed, allowing the extraction of all its poles. It is demonstrated how impurities induce the formation of localized modes which are absent in pristine graphene. The dependence of the spatial modulations over few lattice sites and frequencies of the localized plasmons on the electronic filling and impurity strength is discussed. Furthermore, it is s…
Single-molecule surface enhanced Raman scattering (SM-SERS) is one of the vital applications of plasmonic nanoparticles. The SM-SERS sensitivity critically depends on plasmonic hot-spots created at the vicinity of such nanoparticles. In conventional fluid-phase SM-SERS experiments, plasmonic hot-spots are facilitated by chemical aggregation of nanoparticles. Such aggregation is usually irreversible, and hence, nanoparticles cannot be re-dispersed in the fluid for further use. Here, we show how to combine SM-SERS with plasmon-polariton assisted, reversible assembly of plasmonic nanoparticles at…
Many consumer technologies and scientific methods rely on photodetection of infrared light. We report a Schottky photodetector operating below silicon's band gap energy, through hot carrier injection from a nanoscale metallic absorber. Our design relies on simple CMOS-compatible 'bottom up' fabrication of fractally nanostructured aluminium films. Due to the fractal nature of the nanostructuring, the aluminium films support plasmonically enhanced absorption over a wide wavelength range. We demonstrate two orders of magnitude improvements of responsivity, noise-equivalent-power, and detectivity …
We theoretically investigate equilibrium behaviors and photothermal effects of a flexible plasmonic metamaterial composed of aramid nanofibers and gold nanoparticles. The fiber matrix is considered as an external field to reconfigure a nanoparticle assembly. We find that the heating process tunes particle-particle and fiber-particle interactions, which alter adsorption of nanoparticles on fiber surfaces or clustering in pore spaces. Thus, it is possible to control the nanoparticle self-assembly by laser illumination. Gold nanoparticles strongly absorb radiations and efficiently dissipate absor…
Strong-field photoemission from metal nanostructures enabled fundamental discoveries recently. Here, we deliver theoretical demonstration of the electric field control of electrons in the closest nanoscale vicinity of plasmonic nanoparticles with the help of few-cycle laser waveforms. We analyze the effect of plasmonic resonance on photoemission properties and show that it is only off-resonant nanoparticles that can provide electron control on a true sub-fs timescale.
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…
Graphene monolayers are known to display domains of anisotropic friction with twofold symmetry and anisotropy exceeding 200 percent. This anisotropy has been thought to originate from periodic nanoscale ripples in the graphene sheet, which enhance puckering around a sliding asperity to a degree determined by the sliding direction. Here we demonstrate that these frictional domains derive not from structural features in the graphene, but from self-assembly of atmospheric adsorbates into a highly regular superlattice of stripes with period 4 to 6 nm. The stripes and resulting frictional domains a…
We present an optical investigation of surface plasmon polaritons propagating along nanoscale Au-wires, lithographically defined on GaAs substrates. A two-axis confocal microscope was used to perform spatially and polarization resolved measurements in order to confirm the guiding of surface plasmon polaritons over lengths ranging from $5-20 μm$ along nanowires with a lateral dimension of only $\approx 100 nm$. Finite difference time domain simulations are used to corroborate our experimental observations and highlight the potential to couple proximal quantum dot emitters to propagating plasmon…
There is an increasing scientific and technological interest on the design and implementation of nanoscale sources of quantum light. Here, we investigate the quantum statistics of the light scattered from a plasmonic nanocavity coupled to a mesoscopic ensemble of emitters under low coherent pumping. We present an analytical description of the intensity correlations taking place in these systems, and unveil the fingerprint of plasmon-exciton-polaritons in them. Our findings reveal that plasmonic cavities are able to retain and enhance excitonic nonlinearities even when the number of emitters is…
We discuss two aspects of the plasmofluidic assembly of plasmonic nanostructures at the metal fluid interface. First, we experimentally show how three and four spot evanescent wave excitation can lead to unconventional assembly of plasmonic nanoparticles at the metal fluid interface. We observed that the pattern of assembly was mainly governed by the plasmon interference pattern at the metal fluid interface, and further led to interesting dynamic effects within the assembly. The interference patterns were corroborated by 3D finite difference time domain simulations. Secondly, we show how aniso…
Electron energy-loss spectroscopy (EELS) offers a window to view nanoscale properties and processes. When performed in a scanning transmission electron microscope, EELS can simultaneously render images of nanoscale objects with sub-nanometer spatial resolution and correlate them with spectroscopic information of $\sim10 - 100$ meV spectral resolution. Consequently, EELS is a near-perfect tool for understanding the optical and electronic properties of individual and few-particle plasmonic metal nanoparticles assemblies, which are significant in a wide range of fields. This review presents an ov…
Recent advances in near-field plasmonic metamaterials, such as nanoresonators or transducers, have demonstrated the ability to generate localized fields of high intensity, and thus maintain relatively large nanoscale heat gradients on the order of $10^1-10^2$~K/nm. A plasmonic near-field transducer (NFT) can achieve such large gradients, making population inversion achievable within phononic media. We herein develop a thermal nanomachine composed of a nanoscale phononic laser using InGaAs quantum dot media where an NFT serves as the plasmonic energy source. We show, on demand, the generation o…
Surface plasmon resonances generated in metallic nanostructures can be utilized to tailor electromagnetic fields. The precise spatial arrangement of such structures can result in surprising optical properties that are not found in any naturally occurring material. Here, the designed activity emerges from collective effects of singular components equipped with limited individual functionality. Top-down fabrication of plasmonic materials with a predesigned optical response in the visible range by conventional lithographic methods has remained challenging due to their limited resolution, the comp…
Quantum plasmonics is a rapidly growing field of research that involves the study of the quantum properties of light and its interaction with matter at the nanoscale. Here, surface plasmons - electromagnetic excitations coupled to electron charge density waves on metal-dielectric interfaces or localized on metallic nanostructures - enable the confinement of light to scales far below that of conventional optics. In this article we review recent progress in the experimental and theoretical investigation of the quantum properties of surface plasmons, their role in controlling light-matter interac…
A plasmonic coupled-cavity system, which consists of a quarter-wave coupler cavity, a resonant Fabry-Perot detector nanocavity, and an off-resonant reflector cavity, is used to enhance the localization of surface plasmons in a plasmonic detector. The coupler cavity is designed based on transmission line theory and wavelength scaling rules in the optical regime, while the reflector cavity is derived from off-resonant resonator structures to attenuate transmission of plasmonic waves. We observed strong coupling of the cavities in simulation results, with an 86% improvement of surface plasmon loc…
Surface plasmon polaritons (plasmons) are a combination of light and a collective oscillation of the free electron plasma at metal-dielectric interfaces. This interaction allows sub-wavelength confinement of light, beyond the diffraction limit inherent to dielectric structures. The resulting electromagnetic fields are more intense and the strength of optical interactions between metallic structures and light-sources or detectors can be increased. Plasmons maintain non-classical photon statistics and preserve entanglement on plasmon-assisted transmission through thin, patterned metallic films o…
It is challenging to strongly localize temperature in small volumes because heat transfer is a diffusive process. Here we show how to overcome this limitation using electrodynamic hot spots and interference effects in the regime of continuous-wave (CW) excitation. We introduce a set of figures of merit for the localization of temperature and for the efficiency of the plasmonic photo-thermal effect. Our calculations show that the temperature localization in a trimer nanoparticle assembly is a complex function of the geometry and sizes. Large nanoparticles in the trimer play the role of the nano…
Nanoplasmonic systems combined with optically-active two-dimensional materials provide intriguing opportunities to explore and control light-matter interactions at extreme sub-wavelength lengthscales approaching the exciton Bohr radius. Here, we present room- and cryogenic-temperature investigations of light-matter interactions between an MoSe$_2$ monolayer and individual lithographically defined gold dipole nanoantennas having sub-10 nm feed gaps. By progressively tuning the nanoantenna size, their dipolar resonance is tuned relative to the A-exciton transition in a proximal MoSe$_2$ monolaye…
We design a plasmonic fiber waveguide (PFW) composed of coaxial cylindrical metal-dielectric multilayers in nanoscale, and constitute the corresponding dynamical equations describing the modes of propagation in the PFW with the Kerr nonlinearity in the dielectric layers. The physics is connected to the discrete matrix nonlinear Schrödinger equations, from which the highly confined ring-like solitons in scale of subwavelength are found both for the visible light and the near-infrared light in the self-defocusing condition. Moreover, the confinement could be further improved when increasing the …
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.
Structured light has emerged as an important tool to interrogate and manipulate matter at micron and sub-micron scale. One form of structured light is an optical vortex beam. The helical wavefront of these vortices carry orbital angular momentum which can be transferred to a Brownian colloid. When the colloid is made of metallic nanostructures, such as silver and gold, resonant optical effects play a vital role, and the interaction leads to complex dynamics and assembly. This brief review aims to discuss some recent work on trapping plasmonic colloids with optical vortices and their lattices. …
