A recent study shows that: when a long lifetime particle is positioned near a plasmonic metal nanoparticle, lifetime of plasmon oscillations extends, but, "only" near that long-life particle [PRB 101, 035416 (2020)]. Here, we show that this phenomenon can be utilized for ultrahigh (single-molecule) resolution ultrafast apertureless (scattering) SNOM applications. We use the exact solutions of 3D Maxwell equations. We illuminate a metal-coated silicon tip, a quantum emitter (QE) placed on the tip apex, with a femtosecond laser. The induced near-field in the apex decays rapidly except in the vicinity of the sub-nm-sized QE. Thus, the resolution becomes solely limited by the size of the QE. As positioning of a QE on the tip apex is challenging, we propose the use of a newly-discovered phenomenon; stress-induced defect formation in 2D materials. When a monolayer, e.g., transition metal dichalcogenide (TMD) is transferred to the AFM tip, the tip indentation of 2D TMD originates a defect-center located right at the sharpest point of the tip; that is exactly at its apex. Moreover, the resonance of the defect is tunable via a voltage applied to the tip. Our method can equally be used for background-noise-free nonlinear imaging and for facilitating single-molecule-size chemical manipulation.
Rapid evolutions of microscopic fields govern the majority of elementary excitations in condensed matter and drive microelectronic currents at increasing frequencies. Beyond nominal "radio frequencies", however, access to local electric waveforms remains a challenge. Several imaging schemes resolve sub-wavelength fields up to multi-Terahertz (THz) frequencies - including scanning-probe techniques, electro-optic sampling or recent ultrafast electron microscopy. Yet, various constraints on sample geometries, acquisition speed and maximum fields limit applications. Here, we introduce ubiquitous f…
Non-equilibrium quantum plasmonics in nanoparticle-on-mirror nanocavities
Institute of Fundamental and Frontier Sciences, University of Electronic Science and Technology of China（电子科技大学前沿科学技术研究院）；Photonics Research Centre, Universiti Malaya（马来亚大学光子研究中心）；Nanophotonics Centre, Cavendish Laboratory, Department of Physics, University of Cambridge（剑桥大学物理系卡文迪许实验室纳米光子学中心）
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…
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…
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…
Plasmon-mediated superradiance for molecules around metallic nanospheres was proposed ten years ago. However, its demonstration has not been achieved yet due to the experimental difficulty of positioning molecules, and the theoretical limitation to the enhanced collective rate of low excited molecules. In this Letter, we propose that the ultrafast plasmon-mediated superradiant pulses can be observed with strongly excited methylene blue molecules standing vertically inside gold nanoparticle-on-mirror nanocavities. Our simulations indicate that in this system the molecules could interact with ea…
Electromagnetic coupling between subradiant plasmons and dye molecular excitons analyzed by spectral changes in ultrafast surface-enhanced fluorescence
Health and Medical Research Institute, National Institute of Advanced Industrial Science and Technology (AIST)（产业技术综合研究所健康与医学研究所）；School of Materials Science, Japan Advanced Institute of Science and Technology (JAIST)（日本高级科学技术研究院材料科学学院）
Ultrafast Control of Lifetime in High Q Anisotropic Plasmon Polaritons
Photonics Initiative, Advanced Science Research Center, City University of New York（纽约市立大学先进科学研究中心光子学倡议）；Center for Nano Science and Technology, Fondazione Istituto Italiano di Tecnologia（意大利技术研究院纳米科学与技术中心）；Physics Program, Graduate Center, City University of New York（纽约市立大学研究生院物理学项目）
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…
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…
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…
Polaritons are compositional light-matter quasiparticles that have recently enabled remarkable breakthroughs in quantum and nonlinear optics, as well as in material science. Despite the enormous progress, however, a direct nanometer-scale visualization of polaritons has remained an open challenge. Here, we demonstrate that plasmon-exciton polaritons, or plexcitons, generated by a hybrid system composed of an individual silver nanoparticle and a few-layer transition metal dichalcogenide can be spectroscopically mapped with nanometer spatial resolution using electron energy loss spectroscopy in …
We investigate the non-linear response and energy absorption in bulk silicon irradiated by intense 12-fs near-infrared laser pulses. Depending on the laser intensity, we distinguish two regimes of non-linear absorption of the laser energy: for low intensities, energy deposition and photoionization involve perturbative three-photon transition through the direct bandgap of silicon. For laser intensities near and above 10$^{14}$ W/cm$^2$, corresponding to photocarrier density of order 10$^{22}$ cm$^{-3}$, we find that absorption at near-infrared wavelengths is greatly enhanced due to excitation o…
The ultrafast response of metals to light is governed by intriguing non-equilibrium dynamics involving the interplay of excited electrons and phonons. The coupling between them gives rise to nonlinear diffusion behavior on ultrashort timescales. Here, we use scanning ultrafast thermo-modulation microscopy to image the spatio-temporal hot-electron diffusion in a thin gold film. By tracking local transient reflectivity with 20 nm and 0.25 ps resolution, we reveal two distinct diffusion regimes, consisting of an initial rapid diffusion during the first few picoseconds after optical excitation, fo…
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…
Interference between light waves is one of the widely known phenomena in physics, which is widely used in modern optics, ranging from precise detection at the nanoscale to gravitational-wave observation. Akin to light, both classical and quantum interferences between surface plasmon polaritons (SPPs) have been demonstrated. However, to actively control the SPP interference within subcycle in time (usually less than several femtoseconds in the visible range) is still missing, which hinders the ultimate manipulation of SPP interference on ultrafast time scale. In this paper, the interference bet…
Ultrafast excitation of Bloch plasmon polaritons in hyperbolic metamaterials with an extreme ultra-violet transient grating
Umeå University（于默奥大学）；Elettra Sincrotrone Trieste（的里雅斯特同步辐射中心）；CIC nanoGUNE BRTA（nanoGUNE研究中心）；Ikerbasque, Basque Foundation for Science（伊卡巴斯克，巴斯克科学基金会）；Università degli Studi di Modena e Reggio Emilia（摩德纳和雷焦艾米利亚大学）；Wallenberg Initiative Materials Science for Sustainability（瓦伦堡可持续材料科学倡议）
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…
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…
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. No…
High-quality emission centers in two-dimensional materials are promising components for future photonic and optoelectronic applications. Carbon-enriched hexagonal boron nitride (hBN:C) layers host atom-like color-center (CC) defects with strong and robust photoemission up to room temperature. Placing the hBN:C layers on top of Ag triangle nanoparticles (NPs) accelerate the decay of the CC defects down to 46 ps from their reference bulk value of 350 ps. The ultrafast decay is achieved due to the efficient excitation of the plasmon modes of the Ag NPs by the near field of the CCs. Simulations of…
We propose to enhance the performance of localized plasmon structured illumination microscopy (LP-SIM) via intensity correlations. LP-SIM uses sub-wavelength illumination patterns to encode high spatial frequency information. It can enhance the resolution up to three-fold before gaps in the OTF support arise. For blinking fluorophores or for quantum antibunching an intensity correlation analysis induces higher harmonics of the illumination pattern and enlarges the effective OTF. This enables ultrahigh resolutions without gaps in the OTF support, and thus a fully deterministic imaging scheme. W…
Stimulated Raman scattering (SRS) microscopy allows for high-speed label-free chemical imaging of biomedical systems. The imaging sensitivity of SRS microscopy is limited to ~10 mM for endogenous biomolecules. Electronic pre-resonant SRS allows detection of sub-micromolar chromophores. However, label-free SRS detection of single biomolecules having extremely small Raman cross-sections (~10-30 cm2 sr-1) remains unreachable. Here, we demonstrate plasmon-enhanced stimulated Raman scattering (PESRS) microscopy with single-molecule detection sensitivity. Incorporating pico-Joule laser excitation, b…
