The inclusion of atomic inversion in Raman scattering can significantly alter field dynamics in plasmonic settings. Our calculations show that large local fields and femtosecond pulses combine to yield: (i) population inversion within hot spots; (ii) gain saturation; and (iii) conversion efficiencies characterized by a switch-like transition to the stimulated regime that spans twelve orders of magnitude. While in Raman scattering atomic inversion is usually neglected, we demonstrate that in some circumstances full accounting of the dynamics of the Bloch vector is required.
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…
Stimulated low frequency Raman scattering (SLFRS) in single-crystal diamond films (SCD) with a graphitized layer built-in is investigated. SLFRS process in all studied structures has frequency shift in gigahertz range (5.1-13.2 GHz). Coherent phonon mode excitation at a frequency of several GHz is a result of nonlinear interaction of high-power laser wave with submicron films. SLFRS conversion efficiency and threshold is estimated experimentally. Comparison of the obtained results with data on SLFRS properties in synthetic opal matrixes is made.
We performed non-degenerate pump-probe experiments on a GaAs/AlAs photonic structure. We switched the photonic properties using the optical Kerr effect and free carriers excited by three photon absorption. From these measurements we extracted the non-degenerate Kerr coefficients over a broad wavelength range and we extracted the three photon absorption coefficient for GaAs at three wavelengths in the near infrared. We show that the optical Kerr effect is large enough to switch a cavity resonance with a high \emph{Q} ($Q>1000$) photonic cavity.
The functionalities of a wide range of optical and opto-electronic devices are based on resonance effects and active tuning of the amplitude and wavelength response is often essential. Plasmonic nanostructures are an efficient way to create optical resonances, a prominent example is the extraordinary optical transmission (EOT) through arrays of nanoholes patterned in a metallic film. Tuning of resonances by heating, applying electrical or optical signals has proven to be more elusive, due to the lack of materials that can induce modulation over a broad spectral range and/or at high speeds. Her…
Optically generated electron-hole plasma in high-index dielectric nanostructures was demonstrated as a means of tuning of their optical properties. However, until now an ultrafast operation regime of such plasma driven nanostructures has not been attained. Here, we perform pump-probe experiments with resonant silicon nanoparticles and report on dense optical plasma generation near the magnetic dipole resonance with ultrafast (about 2.5 ps) relaxation rate. Basing on experimental results, we develop an analytical model describing transient response of a nanocrystalline silicon nanoparticle to a…
Coherent anti-Stokes Raman scattering (CARS) and, in particular, femtosecond adaptive spectroscopic techniques (FAST CARS) have been successfully used for molecular spectroscopy and microscopic imaging. Recent progress in ultrafast nanooptics provides flexibility in generation and control of optical near fields, and holds promise to extend CARS techniques to the nanoscale. In this theoretical study, we demonstrate ultrafast subwavelentgh control of coherent Raman spectra of molecules in the vicinity of a plasmonic nanostructure excited by ultrashort laser pulses. The simulated nanostructure de…
We describe an ultrafast time resolved pump-probe spectroscopy setup aimed at studying the switching of nanophotonic structures. Both fs pump and probe pulses can be independently tuned over broad frequency range between 3850 and 21050 cm$^{-1}$. A broad pump scan range allows a large optical penetration depth, while a broad probe scan range is crucial to study strongly photonic crystals. A new data acquisition method allows for sensitive pump-probe measurements, and corrects for fluctuations in probe intensity and pump stray light. We observe a tenfold improvement of the precision of the setu…
Time-resolved femtosecond stimulated Raman spectroscopy (FSRS) is a powerful tool for investigating ultrafast structural and vibrational dynamics in light absorbing systems. However, the technique generally requires exposing a sample to high laser pulse fluences and long acquisition times to achieve adequate signal-to-noise ratios. Here, we describe a timeresolved FSRS instrument built around a Yb ultrafast amplifier operating at 200 kHz, and address some of the unique challenges that arise at high repetition-rates. The setup includes detection with a 9 kHz CMOS camera and an improved dual-cho…
Future technologies underpinning high-performance optical communications, ultrafast computations and compact biosensing will rely on densely packed reconfigurable optical circuitry based on nanophotonics. For many years, plasmonics was considered as the only available platform for nanoscale optics, but the recently emerged novel field of Mie resonant metaphotonics provides more practical alternatives for nanoscale optics by employing resonances in high-index dielectric nanoparticles and structures. In this mini-review we highlight some recent trends in the physics of dielectric Mie-resonant na…
Diffusion of heat in metals is a fundamental process which is crucial for a variety of applications of metal nanostructures. Surprisingly, however, {\em ultrafast} heat diffusion received only limited attention so far. Here, we show that heat diffusion can be made faster than $e-ph$ energy transfer rate, in which case, it dominates the spatio-temporal dynamics of the temperature. This enables the metals to overcome the conventional limitations of the nonlinear optical response of materials - it can be simultaneously fast and strong. As a specific example, we identify the underlying (femtosecon…
Momentum microscopy of ultrafast electron emission from a strongly driven optical nanoantenna
Carl von Ossietzky Universität Oldenburg（奥尔登堡卡尔·冯·奥西茨基大学）；ELI ALPS, The Extreme Light Infrastructure ERIC（ELI ALPS，极端光基础设施ERIC）；Leibniz Institute of Photonic Technology（莱布尼兹光子技术研究所）；Universität Würzburg（维尔茨堡大学）；Friedrich-Schiller-Universität Jena（耶拿弗里德里希·席勒大学）；HUN-REN Wigner Research Center for Physics（匈牙利科学院Wigner物理研究中心）
We demonstrate theoretically that ultrafast heating of metal nanoparticles by the laser pulse should lead to the generation of coherent terahertz (THz) radiation during the heat redistribution process. It is shown that after the femtosecond laser pulse action the time-dependent gradient of the electronic temperature induces low-frequency particle polarization with the characteristic timescale of about fractions of picosecond. In the case of the directed metallic pattern, the THz pulse waveform can be controlled by changing geometry of the individual particle. The generation mechanism proposed …
We present multi-color imaging by stimulated Raman scattering (SRS) enabled by an ultrafast fiber-based light source with integrated amplitude modulation and frame-to-frame wavelength tuning. With a relative intensity noise level of -153.7 dBc/Hz at 20.25 MHz the light source is well suited for SRS imaging and outperforms other fiber-based light source concepts for SRS imaging. The light source is tunable in under 5 ms per arbitrary wavelength step between 700 cm$^{-1}$ and 3200 cm$^{-1}$, which allows for addressing Raman resonances from the fingerprint to the CH-stretch region. Moreover, the…
Here we describe an optical method to determine the dynamics of optically excited carriers in nanostructured composite samples. By combining pump-probe time-resolved reflectivity with scattering measurements, we extract the characteristic times for charge carrier evolution. We use the 3D Maxwell-Garnett formulae, modified to include the Drude optical response, to model the results. The method, applied to hydrogenated amorphous silicon containing crystalline silicon nanoparticles, showed that the recombination times in the nanocrystals and in the matrix were ~4.9 ps and ~22 ps, respectively. Th…
We report and propose a simple scheme to achieve efficient and fast coherent population transfer (CPT) by utilizing either a nonlinearly chirped Gaussian shaped few-cycle laser pulse or an unchirped sinc-shaped few-cycle laser pulse. The proposed scheme is shown to be fairly robust against the variation of the laser parameters such as temporal pulse width, chirp rates, carrier envelope phases and Rabi frequencies. We find that compared to the so-called stimulated Raman adiabatic passage (STIRAP) technique, our scheme for complete population transfer with few-cycle Gaussian shaped laser pulses …
Nonlinear nanophotonics is a rapidly developing field with many useful applications for a design of nonlinear nanoantennas, light sources, nanolasers, sensors, and ultrafast miniature metadevices. A tight confinement of the local electromagnetic fields in resonant photonic nanostructures can boost nonlinear optical effects, thus offering versatile opportunities for subwavelength control of light. To achieve the desired functionalities, it is essential to gain flexible control over the near- and far-field properties of nanostructures. Thus, both modal and multipolar analyses are widely exploite…
We investigate - both experimentally and theoretically - the inelastic interaction between fast electrons and the electromagnetic field scattered by metallic apertures and nanostructures on dielectric membranes using photon induced near-field electron microscopy. The experiments - performed in a high brightness ultrafast transmission electron microscope - on gold apertures on silicon nitride membranes reveal strong modulations of the electron-light coupling strength. We demonstrates that this effect results from the combined action of the electric field scattered by the aperture edges and the …
As a key component for next-generation wireless communications (6G and beyond), terahertz (THz) electronic oscillators are being actively developed. Precise and dynamic phase control of ultrafast THz waveforms is essential for high-speed beam steering and high-capacity data transmission. However, measurement of such ultrafast dynamic process is beyond the scope of electronics due to the limited bandwidth of the electrical measuring instruments. Here we surpass this limit by applying photonic technology. Using a femtosecond laser, we generate offset-free THz pulses to phase-lock the electronic …
Ultrashort high-energy pulses at wavelengths longer than 1 $μ$m are nowadays desired for a vast variety of applications in ultrafast and strong-field physics. To date, the main answer to the wavelength tunability for energetic, broadband pulses still relies on optical parametric amplification (OPA), which often requires multiple and complex stages, may feature imperfect beam quality and has limited conversion efficiency into one of the amplified waves. In this work, we present a completely different strategy to realize an energy-efficient and scalable laser frequency shifter. This relies on th…
A significant interest in combining plasmonics and magnetism at the nanoscale gains momentum in both photonics and magnetism sectors that are concerned with the resonant enhancement of light-magnetic-matter interaction in nanostructures. These efforts result in a considerable amount of literature, which is difficult to collect and digest in limited time. Furthermore, there is insufficient exchange of results between the two research sectors. Consequently, the goal of this review paper is to bridge this gap by presenting an overview of recent progress in the field of magneto-plasmonics from two…
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…
Nanoscale semiconductor lasers have been developed recently using either metal, metallo-dielectric or photonic crystal nanocavities. While the technology of nanolasers is steadily being deployed, their expected performance for on-chip optical interconnects is still largely unknown due to a limited understanding of some of their key features. Specifically, as the cavity size is reduced with respect to the emission wavelength, the stimulated and the spontaneous emission rates are modified, which is known as the Purcell effect in the context of cavity quantum electrodynamics. This effect is expec…
The chaotic nature of x-ray free-electron-laser pulses is a major bottleneck that has limited the joint temporal and spectral resolution of spectroscopic measurements. We show how to use the stochastic x-ray field statistics to overcome this difficulty by correlation signals averaged over independent pulse realizations. No control is required over the spectral phase of the pulse, enabling immediate application with existing, noisy x-ray free-electron-laser pulses. The proposed stimulated Raman technique provides the broad observation bandwidth and high time-frequency resolution needed for the …
In the Kapitza-Dirac effect, atoms, molecules, or swift electrons are diffracted off a standing wave grating of the light intensity created by two counter-propagating laser fields. In ultrafast electron optics, such a coherent beam splitter offers interesting perspectives for ultrafast beam shaping. Here, we study, both analytically and numerically, the effect of the inclination angle between two laser fields on the diffraction of pulsed, low-energy electron beams. For sufficiently high light intensities, we observe a rich variety of complex diffraction patterns. These do not only reflect inte…
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…
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…
An important vision of modern magnetic research is to use antiferromagnets as controllable and active ultrafast components in spintronic devices. Hematite is a promising model material in this respect because its pronounced Dzyaloshinskii-Moriya interaction leads to the coexistence of antiferromagnetism and weak ferromagnetism. Here, we use femtosecond laser pulses to drive terahertz spin currents from hematite into an adjacent Pt layer. We find two contributions to the generation of the spin current with distinctly different dynamics: the impulsive stimulated Raman scatting that relies on the…
Since the advent of atom laser-cooling, trapping or cooling natural molecules has been a long standing and challenging goal. Here, we demonstrate a method for laser-trapping molecules that is radically novel in its configuration, in its underlined physical dynamics and in its outcomes. It is based on self-optically spatially-nanostructured high pressure molecular hydrogen confined in hollow-core photonic-crystal-fibre. An accelerating molecular-lattice is formed by a periodic potential associated with Raman saturation except for a 1-dimentional array of nanometer wide and strongly-localizing s…
Spatio-temporal shaping of electron beams is a bold frontier in electron microscopy, enabling new routes toward spatial-resolution enhancement, selective probing, low-dose imaging and faster data acquisition. Over the last decade, shaping methods evolved from passive phase plates to low-speed electrostatic and magnetostatic displays. Recently, higher shaping speed and flexibility have become feasible by the advent of ultrafast electron microscopy, embodying a swift change of paradigm that relies on using light to control free electrons. Here, we experimentally demonstrate that arbitrary transv…
We present a theoretical study of temporal, spectral, and spatial reshaping of intense, ultrafast x-ray pulses propagating through a resonant medium. Our calculations are based on the solution of a 3D time-dependent Schrödinger-Maxwell equation, with the incident x-ray photon energy on resonance with the core-level 1s-3p transition in neon. We study the evolution of the combined incident and medium-generated field, including the effects of stimulated emission, absorption, ionization and Auger decay, as a function of the input pulse energy and duration. We find that stimulated Raman scattering …
High-harmonic generation (HHG) in condensed-matter systems is both a source of fundamental insight into quantum electron motion and a promising candidate to realize compact ultraviolet and ultrafast light sources. Here we argue that the large light intensity required for this phenomenon to occur can be reached by exploiting localized plasmons in conducting nanostructures. In particular, we demonstrate that doped graphene nanostructures combine a strong plasmonic near-field enhancement and a pronounced intrinsic nonlinearity that result in efficient broadband HHG within a single material platfo…
