We discuss finite-difference time-domain simulations of femtosecond pulses interacting with silver nanowires and nanoparticles. We show how localized hot spots near the metal surfaces can be generated and controlled in a spatiotemporal manner. The control is made possible by chirping the pulses such that the effective frequency passes through surface plasmon resonances associated with different spatial regions of the nanostructure over the course of time. The response of such nanostructures to chirped pulses could provide a novel means of encoding or decoding optical signals.
We report on an experimental measurement of the pulse front tilt (PFT) of spatiotemporally focused femtosecond laser pulses in the focal plane in both air and bulk transparent materials, which is achieved by examination of the interference pattern between the spatiotemporally focused pulse and a conventional focused reference pulse as a function of time delay between the two pulses. Our simulation results agree well with the experimental observations.
Femtosecond laser micromachining provides high precision and less thermal diffusion in surface structuring as a result of the ultrashort temporal duration and ultrahigh peak intensity of the femtosecond laser pulses. To increase the throughput of surface patterning, the focal spot size can be expanded with loose focusing, which, however, could lead to nonlinear self-focusing of the pulses when the pulses propagate in air. We solve the problem by use of spatiotemporally focused femtosecond laser pulses for ablation of metal surfaces, which gives rise to improved surface quality as compared with…
We report on experimental observations of formation and evolution of transient plasma produced in fused silica glass with spatiotemporally focused (STF) femtosecond laser pulses using a pump-probe shadow imaging technique. Surprisingly, the observation shows that the track of the plasma is significantly curved, which is attributed to an asymmetric density distribution of the transient plasma produced in the focal volume caused by the pulse front tilt of the STF laser field.
We observe that focusing a femtosecond laser beam simultaneously chirped in time and space domains in glass can efficiently suppress the optical aberration caused by the refractive index mismatch at the interface of air and the glass sample. We then demonstrate three dimensional microprocessing in glass with a nearly invariant spatial resolution for a large range of penetration depth between 0.25 mm and 9 mm without any aberration correction.
We have developed a single-shot imaging technique that can capture ultrafast events occurring on femtosecond to picosecond time scales. The technique is based on an optical pump-probe method, in which multiple time-delayed femtosecond pulses simultaneously probe a pump-excited sample. Here we use two sets of 2-by-2 mirror arrays for spatial/temporal division and routing of multiple probe pulses. This single-shot scheme is successfully applied to capture femtosecond ionization fronts propagating at the speed of light in air, as well as laser-induced ablation of solid targets.
The performance of fiber mode-locked lasers is limited due to the high nonlinearity induced by the spatial confinement of the single-mode fiber core. To massively increase the pulse energy of the femtosecond pulses, amplification is obtained outside the oscillator. Recently, spatiotemporal mode-locking has been proposed as a new path to fiber lasers. However, the beam quality was either highly multimode and/or with low pulse energy. Here we present an approach to reach high energy per pulse directly in the mode-locked multimode fiber oscillator with a near single-mode output beam. Our approach…
We use ultrafast pump-probe transmission spectroscopy to measure the electronic relaxation time for electrons in cobalt nanoparticles embedded on glass substrate using femtosecond laser pulses. We found that the plasmon excitation is inhomogenously broadening with a fast excitation time of 23 fs. and a plasmonic relaxation time of 97fs. The femtosecond laser pulses used in this experiment were come from a Ti:Sapphire resonator that uses a self-mode-locking mechanism based on the nonlinear Kerr effect. The pulses were found to have repetition rate of 103.52MHz with a pulse width of 64.5 fs at F…
We propose a novel approach for efficient tuning of optical properties of a high refractive index subwavelength nanoparticle with a magnetic Mie-type resonance by means of femtosecond laser irradiation. This concept is based on ultrafast photo-injection of dense (>10^20 cm^-3) electron-hole plasma within such nanoparticle, drastically changing its transient dielectric permittivity. This allows to manipulate by both electric and magnetic nanoparticle responses, resulting in dramatic changes of its scattering diagram and scattering cross section. We experimentally demonstrate 20 % tuning of refl…
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…
We measure the detailed spatiotemporal profiles of femtosecond laser pulses in the infrared wavelength range λ=2.5-11μm, and the absolute nonlinear response of major air constituents (N2, O2, and Ar) over this range. The spatiotemporal measurements reveal wavelength-dependent pulse front tilt and temporal stretching in the infrared pulses.
We experimentally demonstrate energy exchange between a delay-tuned femtosecond beam and two delay-fixed ones as they spatiotemporally overlapped and experienced filamentation in air. The energy exchange process in the relative time delay is dramatically elongated up to 40 ps in the presence of plasma grating, indicating that filamentary beams coupling may be an effective method for filament control.
Ultrafast X-ray imaging provides high resolution information on individual fragile specimens such as aerosols, metastable particles, superfluid quantum systems and live biospecimen, which is inaccessible with conventional imaging techniques. Coherent X-ray diffractive imaging, however, suffers from intrinsic loss of phase, and therefore structure recovery is often complicated and not always uniquely-defined. Here, we introduce the method of in-flight holography, where we use nanoclusters as reference X-ray scatterers in order to encode relative phase information into diffraction patterns of a …
Using SEA TADPOLE with micrometer-range spatial and femtosecond-range temporal resolution, we report the first direct spatiotemporal measurements of ultrashort Bessel-X pulses. We demonstrate their propagation invariance and superluminal velocity and verify our results with simulations
The use of structured ultrashort pulses with coupled spatiotemporal properties is emerging as a key tool for ultrafast manipulation. Ultrafast vector beams are opening exciting opportunities in different fields such as microscopy, time-resolved imaging, nonlinear optics, particle acceleration or attosecond science. Here, we implement a technique for the full characterization of structured time-dependent polarization light waveforms with spatiotemporal resolution, using a compact twofold spectral interferometer, based on in-line bulk interferometry and fibre-optic coupler assisted interferometr…
Modulation of the optical index by means of atomic and material resonances provides a basis for controlling light propagation in natural and artificially fabricated materials. In addition, recent advances in the tuning of spatiotemporal couplings of ultrashort laser pulses have enabled almost arbitrary control over the group velocity of light. Here, using femtosecond time-resolved microscopy and numerical calculations, we investigate the spatiotemporal dynamics of a surface plasmon polariton wave packet (SPP WP) that interacts with a plasmonic nanocavity. The nanocavity consists of metal-insul…
An influence of pass-through optics on femtosecond laser pulse filamentation in ambient air is analyzed for the first time both experimentally and numerically. Propagation of high-power femtosecond laser pulse through solid optical elements introduces spatiotemporal phase modulation due to the Kerr effect. This modulation may have a strong ef-fect on the pulse filamentation in air. We demonstrated that the phase modulation obtained in the thin pass-through dielectric plate reduces the distance to the filament onset and increases the plasma channel length
Raman spectroscopic characterization of crater walls formed upon single-shot high energy femtosecond laser irradiation of dimethacrylate polymer doped with plasmonic gold nanorods
In this work we use femtosecond laser pulses of 800 nm wavelength to excite and characterize the multiphoton luminescence emission of single gold nanoparticles. For excitation with 100 fs laser pulses we observe a two and three photon emission dominated by radiative electron hole pair recombination, while the emission is caused by radiative plasmon decay for excitation with 500 fs pulses. For single gold nanorods with different aspect ratios, we study the interplay between the particle plasmon and electron hole pairs, which enables us to develop a quantitative model to fully describe the two a…
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 …
In this work we present a scheme to control the optical dipole trap potential in an N-type four-level atomic system by using chirped femtosecond Gaussian pulses. The spatial size of the trap can be well controlled by tuning the beam waist of the Gaussian pulse and the detuning frequency. The trapping potential splits with increasing Rabi frequency about the center of the trap, a behavior analogous to the one observed experimentally in the context of trapping of nanoparticles with femtosecond pulses. An attempt is made to explain the physics behind this phenomenon by studying the spatial probab…
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…
Intrinsic to the process of high-order harmonic generation is the creation of plasma and the resulting spatiotemporal distortions of the driving laser pulse. Inside a high finesse cavity where the driver pulse and gas medium are reused, this can lead to optical bistability of the cavity-plasma system, accumulated self-phase modulation of the intracavity pulse, and coupling to higher order cavity modes. We present an experimental and theoretical study of these effects and discuss their implications for power scaling of intracavity high-order harmonic generation and extreme ultraviolet frequency…
We present the effect of a nanostructured surface on the emission of ions and electrons from intense (5-36 Petwatt per sq.cm) femtosecond laser produced plasmas. Electrons from optically polished copper targets coated with copper nanoparticles (CuNP) are observed to be hotter than those from uncoated polished targets. A nearly two-fold enhancement is observed for ions in the range 14-74 keV, while ion yield decreases by a factor of 2 in the 74-2000 keV range. The total ion yields measured using a large area Faraday cup are more from CuNP targets than those from polished Cu targets, indicating …
By using a powerful reductive perturbation technique, or a multiscale analysis, a generic Kadomtsev-Petviashvili evolution equation governing the propagation of femtosecond spatiotemporal optical solitons in quadratic nonlinear media beyond the slowly varying envelope approximation is put forward. Direct numerical simulations show the formation, from adequately chosen few-cycle input pulses, of both stable line solitons (in the case of a quadratic medium with normal dispersion) and of stable lumps (for a quadratic medium with anomalous dispersion). Besides, a typical example of the decay of th…
This letter is to pave the way towards the demonstration of spatiotemporal similariton pulses evolution in passive multimode fibers with Raman amplification. We present numerically these issues in a graded-index and step-index multimode fibers and provide a first look at the complex spatiotemporal dynamics of similariton pulses. The results showed that the similariton pulses can be generated in both multimode fibers. The temporal and the spectral evolution of the pulses can be characterized as parabolic shapes with linear chirp and kW peak power. By compressed these, high energy femtoseconds p…
Numerous techniques have been demonstrated for effective generation of orbital angular momentum-carrying radiation, but intracavity generation of continuously tunable pulses in the femtosecond regime remains challenging. Even if such a creation was realized, the generated pulses, like all pulses in reality, are complex and transitory objects that can only be comprehensively characterized via multidimensional spaces. An integrated lasing system that generates pulses while simultaneously quantifies them can achieve adaptive pulse tailoring. Here, we report a femtosecond pulse scope that unifies …
Ultra-high intensity femtosecond lasers at focus are now routinely used for relativistic motion of charged particles with peak intensities over 10^18W/cm^2. Such high-field experiments are very sensitive to the value of the peak intensity. Therefore, precise knowledge of the pulse intensity is a key prerequisite for the correct interpretation of experimental data. Accurate measurement of energy, spectral and spatial profiles being well established, peak intensity evaluation then only requires the determination of the spatiotemporal Strehl ratio. Here I propose a new method based on a simple an…
We present a method of rendering aerial and volumetric graphics using femtosecond lasers. A high-intensity laser excites a physical matter to emit light at an arbitrary 3D position. Popular applications can then be explored especially since plasma induced by a femtosecond laser is safer than that generated by a nanosecond laser. There are two methods of rendering graphics with a femtosecond laser in air: Producing holograms using spatial light modulation technology, and scanning of a laser beam by a galvano mirror. The holograms and workspace of the system proposed here occupy a volume of up t…
We propose a new concept for generation of ultrashort pulses based on transient plasmonic resonance in nanoparticle composites. Photoionization and free-carriers plasma change the susceptibility of nanoparticles on a few-femtosecond scale. This results in a narrow time window during the pump pulse duration when the system is in plasmonic resonance, accompanied by a short burst of the local field. During this process, frequency-tunable few-fs pulses are generated. We elucidate the details of the above mechanism, and investigate the influences of different contributing processes.
Monitoring of nanoplasmonics-assisted deuterium production in a polymer seeded with resonant Au nanorods using in situ femtosecond laser induced breakdown spectroscopy
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…
We propose a novel type of tunable Yagi-Uda nanoantenna composed of metal-dielectric (Ag-Ge) core-shell nanoparticles. We show that, due to the combination of two types of resonances in each nanoparticle, such hybrid Yagi-Uda nanoantenna can operate in two different regimes. Besides the conventional nonresonant operation regime at low frequencies, characterized by highly directive emission in the forward direction, there is another one at higher frequencies caused by hybrid magneto-electric response of the core-shell nanoparticles. This regime is based on the excitation of the van Hove singula…
Shaping electron beams with the cycles of light provides femtosecond and attosecond time resolution in electron microscopy and enables fundamental quantum-coherent measurements. However, efficient light-electron control requires a prolonged interaction between the two beams for cascaded transfer of photon energy and momentum to the freely propagating electrons. Here we report the use of traveling evanescent terahertz waves to achieve velocity matching and thereby high acceleration gradients both in space and in time. With experiment and simulations, we demonstrate attosecond streaking, tempora…
Diffraction-before-destruction imaging with single ultrashort X-ray pulses has the potential to visualise non-equilibrium processes, such as chemical reactions, at the nanoscale with sub-femtosecond resolution in the native environment without the need of crystallization. Here, a nanospecimen partially diffracts a single X-ray flash before sample damage occurs. The structural information of the sample can be reconstructed from the coherent X-ray interference image. State-of-art spatial resolution of such snapshots from individual heavy element nanoparticles is limited to a few nanometers. Furt…
A dramatic spectral modulation of third-order harmonic (TH) emission generated in a near in- frared femtosecond (fs) pulse filamentation, assisted by a two-dimensional plasma grating formed by two pump femtosecond pulses, is experimentally demonstrated when their spatiotemporal overlap is achieved. It is mainly attributed to strong cross-phase modulation induced by the fundamental wave of the probe pulse and two pump ones. The delay dynamic of TH spectra indicates the influence of two retarded nonlinear responses on the TH generation. The dependences of TH generation on the energies of probe a…
Hybrid nanophotonics based on metal-dielectric nanostructures unifies the advantages of plasmonics and all-dielectric nanophotonics providing strong localization of light, magnetic optical response and specifically designed scattering properties. Here we demonstrate a novel approach for fabrication of ordered hybrid nanostructures via femtosecond laser melting of asymmetrical metal-dielectric (Au-Si) nanoparticles created by lithographical methods. The approach allows selective reshaping of the metal components of the hybrid nanoparticles without affecting dielectric ones. We apply the develop…
Ultrafast imaging is essential in physics and chemistry to investigate the femtosecond dynamics of nonuniform samples or of phenomena with strong spatial variations. It relies on observing the phenomena induced by an ultrashort laser pump pulse using an ultrashort probe pulse at a later time. Recent years have seen the emergence of very successful ultrafast imaging techniques of single non-reproducible events with extremely high frame rate, based on wavelength or spatial frequency encoding. However, further progress in ultrafast imaging towards high spatial resolution is hampered by the lack o…
Recent developments in the area of resonant dielectric nanostructures has created attractive opportunities for the concentrating and manipulating light at the nanoscale and the establishment of new exciting field of all-dielectric nanophotonics. Transition metal dichalcogenides (TMDCs) with nanopatterned surfaces are especially promising for these tasks. Still, the fabrication of these structures requires sophisticated lithographic processes, drastically complicating application prospects. To bridge this gap and broaden the application scope of TMDC nanomaterials, we report here femtosecond la…
Progress in electron-beam spectroscopies has recently enabled the study of optical excitations with combined space, energy and time resolution in the nanometer, millielectronvolt and femtosecond domain, thus providing unique access into nanophotonic structures and their detailed optical responses. These techniques rely on $\approx$ 1-300 keV electron beams focused at the sample down to sub-nanometer spots, temporally compressed in wavepackets a few femtoseconds long, and in some cases controlled by ultrafast light pulses. The electrons undergo energy losses and gains, also giving rise to catho…
Understanding the differences between photon-induced and plasmon-induced hot electrons is essential for the construction of devices for plasmonic energy conversion. The mechanism of the plasmonic enhancement in photochemistry, photocatalysis, and light-harvesting and especially the role of hot carriers is still heavily discussed. The question remains, if plasmon-induced and photon-induced hot carriers are fundamentally different, or if plasmonic enhancement is only an effect of field concentration producing these carriers in greater numbers. For the bulk plasmon resonance, a fundamental differ…
We image the field enhancement at Ag nanostructures using femtosecond laser pulses with a center wavelength of 1.55 micrometer. Imaging is based on non-linear photoemission observed in a photoemission electron microscope (PEEM). The images are directly compared to ultra violet PEEM and scanning electron microscopy (SEM) imaging of the same structures. Further, we have carried out atomic scale scanning tunneling microscopy (STM) on the same type of Ag nanostructures and on the Au substrate. Measuring the photoelectron spectrum from individual Ag particles shows a larger contribution from higher…
We study the excitation dynamics of Fano resonance within the classical model framework of two linear coupled oscillators. An exact solution for the model with a damped harmonic force is obtained. The details of growth a Fano profile under the harmonic excitation is shown. For incident ultra-wideband pulse, the reaction of a system becomes universal and coincides with the time-dependent response function. The results of numerical calculations clarify two alternative ways for experimental measurement of the complete characteristics of a system: direct observation of the system response to a mon…
Influence of Inter-Pulse Delay and Geometric Constraints on Damage and Optical Characteristics in thin Metal Targets Irradiated by Double Ultrashort Laser Pulses
Institute of Electronic Structure and Laser (IESL), Foundation for Research and Technology (FORTH)（电子结构与激光研究所，研究与技术基金会）
We present a novel approach for tailoring the laser induced surface topography upon femtosecond-fs pulsed laser irradiation. The method employs spatially controlled double fs laser pulses to actively regulate the hydrodynamic microfluidic motion of the melted layer that gives rise to the structures formation. The pulse train used, in particular, consists of a previously unexplored spatiotemporal intensity combination including one pulse with Gaussian and another with periodically modulated intensity distribution created by Direct Laser Interference Patterning (DLIP). The interpulse delay is ap…
