Ultrafast lasers are ideal tools to process transparent materials because they spatially confine the deposition of laser energy within the material's bulk via nonlinear photoionization processes. Nonlinear propagation and filamentation were initially regarded as deleterious effects. But in the last decade, they turned out to be benefits to control energy deposition over long distances. These effects create very high aspect ratio structures which have found a number of important applications, particularly for glass separation with non-ablative techniques. This chapter reviews the developments of in-volume ultrafast laser processing of transparent materials. We discuss the basic physics of the processes, characterization means, filamentation of Gaussian and Bessel beams and provide an overview of present applications.
A comparative experimental and theoretical investigation is presented that centres on the effects of structuring black silicon surfaces with linearly, circularly and azimuthally polarized laser pulses under SF6 ambient atmosphere. It is shown that the asymmetric elliptical micro-cone formations induced by linearly polarized beams result in variable light absorption due to their spatial asymmetry. By contrast, the use of azimuthally polarized beams leads to an omni-directionality of the elliptical cone orientation which is dependent on the local electric field during laser scanning. The locally…
We present here a nanosecond laser ablation of Si(111) wafer with diffraction-free (Bessel-$J_0$) beams. First, the Axicon a conical shaped optical element for beam shaping is characterized with a visible and infrared light sources. Then, ablation profiles are obtained with Bessel beams generated for $α=1^{\circ}$ and $α=20^{\circ}$ base angles, then they are characterized via a Scanning Electron, an Atomic Force and an Optical Interferometric Microscopes. Experimental results compared with theoretical predictions obtained by using Bessel functions. Results show that Bessel beams give possibil…
In the past few years, phase-change materials have become increasingly important in nano-photonics and optoelectronics. The advantages of sizeable optical contrast between phases and the additional degree of freedom from phase switching have been the driving force. From multilevel reflectance to dynamic nanoprinting and structural colors, phase-change materials have achieved outstanding results with prospects for real-world applications. The local crystallization/amorphization of phase-change materials and the corresponding reflectance tunning by the crystallized/amorphized region size have po…
An epsilon-near-zero-based nonlinear platform for ultrafast re-writable holography
University of Ottawa（渥太华大学）；Tampere University（坦佩雷大学）；University of Rochester（罗切斯特大学）；Yale University（耶鲁大学）；Technische Universität Darmstadt（达姆施塔特工业大学）
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 …
Synthetic chiral light enables ultrafast and highly efficient imaging of molecular chirality. Unlike standard circularly polarized light, the handedness of synthetic chiral light does not rely on the spatial structure of the light field: it is encoded locally, in the chiral trajectory that the tip of the electric-field vector draws in time, at each point in space. Being locally chiral, already within the electric-dipole approximation, synthetic chiral light is a highly efficient chiral photonic reagent. Synthetic chiral light that is locally and globally chiral allows us to selectively quench …
Ultrafast Bessel beams demonstrate a significant capacity of structuring transparent materials with high degree of accuracy and exceptional aspect ratio. The ability to localize energy on the nanometer scale (bypassing the 100 nm milestone) makes them ideal tools for advanced laser nanoscale processing on surfaces and in the bulk. This allows to generate and combine micron and nano-sized features into hybrid structures that show novel functionalities. Their high aspect ratio and the accurate location can equally drive an efficient material modification and processing strategy on large dimensio…
We report on a chiral nanostructure, which we term a "butterfly nanoantenna," that, when used in a metasurface, allows the direct conversion of a linearly polarized beam into a nonlinear optical far-field of arbitrary complexity. The butterfly nanoantenna exhibits field enhancement in its gap for every incident linear polarization, which can be exploited to drive nonlinear optical emitters within the gap, for the structuring of light within a frequency range not accessible by linear plasmonics. As the polarization, phase and amplitude of the field in the gap are highly controlled, nonlinear em…
Ultrafast lasers have revolutionized material processing, opening a wealth of new applications in many areas of science. A recent technology that allows the cleaving of transparent materials via non-ablative processes is based on focusing and translating a high-intensity laser beam within a material to induce a well-defined internal stress plane. This then enables material separation without debris generation. Here, we use a non-diffracting beam engineered to have a transverse elliptical spatial profile to generate high aspect ratio elliptical channels in glass of dimension 350 nm x 710 nm, an…
We report on the broadband transient optical response from anisotropic nanobrick amorphous silicon particles, exhibiting Mie-type resonances. A quantitative model is developed to identify and disentangle the three physical processes that govern the ultrafast changes of the nanobrick optical properties, namely two-photon absorption, free-carrier relaxation, and lattice heating. We reveal a set of operating windows where ultrafast all-optical modulation of transmission is achieved with full return to zero in 20 ps. This is made possible due to the interplay between the competing nonlinear proces…
Femtosecond laser ablation has been demonstrated to be a versatile tool to produce micro/nanoscale features with high precision and accuracy. However, the use of high laser fluence to increase the ablation efficiency usually results in unwanted effects, such as redeposition of debris, formation of recast layer and heat-affected zone in or around the ablation craters. Here we circumvent this limitation by exploiting a thin frost layer with a thickness of tens of microns, which can be directly formed by the condensation of water vapor from the air onto the exposed surface whose temperature is be…
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…
Electrodes with higher transparency that can also align liquid crystals (LCs) are of high importance for improved costs and energy consumption of LC displays. Here we demonstrate for the first time alignment of liquid crystals on femtosecond laser nanostructured indium tin oxide (ITO) coated glass exhibiting also higher transparency due to the less interface reflections. The nano paterns were created by fs laser directlly on ITO films without any additional spin coating materials or lithography procces. Nine regions of laser-induced nanostructures were fabricated with different alignment orien…
The industrial maturity of ultrashort pulsed lasers has triggered the development of a plethora of material processing strategies. Recently, the combination of these remarkable temporal pulse properties with advanced structured light concepts has led to breakthroughs in the development of novel laser application methods, which will now gradually reach industrial environments. We review the efficient generation of customized focus distributions from the near infrared down to the deep ultraviolet, e.g., based on non-diffracting beams and 3D-beam splitters, and demonstrate their impact for micro-…
While ultrafast laser welding is an appealing technique for bonding transparent workpieces, it is not applicable for joining silicon samples due to nonlinear propagation effects which dramatically diminishes the possible energy deposition at the interface. We demonstrate that these limitations can be circumvented by local absorption enhancement at the interface thanks to metallic nanolayer deposition. By combining the resulting exalted absorption with filament relocation during ultrafast laser irradiation, silicon samples can be efficiently joined. Shear joining strengths >4 MPa are obtained f…
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…
The full control of the fundamental photophysics of nanosystems at frequencies as high as few THz is key for tunable and ultrafast nano-photonic devices and metamaterials. Here we combine geometrical and ultrafast control of the optical properties of halide perovskite nanoparticles, which constitute a prominent platform for nanophotonics. The pulsed photoinjection of free carriers across the semiconducting gap leads to a sub-picosecond modification of the far-field electromagnetic properties that is fully controlled by the geometry of the system. When the nanoparticle size is tuned so as to ac…
Distinguishing between the left- and right-handed versions of a chiral molecule (enantiomers) is vital, but also inherently difficult. Traditional optical methods using elliptically or circularly polarized light rely on weak linear effects which arise beyond the electric-dipole approximation, posing major limitations for time resolving ultrafast chiral molecular dynamics. Here we show how, by tilting the plane of polarization of an ultrashort burst of intense elliptically polarized light, towards its propagation direction, we can turn the light field into a highly efficient chiro-optical tool.…
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 emergence of strong-field nanoplasmonics brings extreme laser field-matter interaction into the realm of nanoscale science, unveiling exciting new physics. Highly nonlinear interaction is enabled by tightly confined electric fields in nanoplasmonic structures, permitting use of optical fields from low-power laser oscillators. Here, we report the first demonstration of visible 517nm third harmonic generation in ultracompact nanoplasmonic waveguides on a silicon-on-insulator platform at an unprecedented conversion efficiency of ~10^{-5}. Exponential growth of broadband white light generation…
Metasurfaces control optical wavefronts via arrays of nanoscale resonators laid out across a surface. When combined with III-V semiconductors with strong optical nonlinearities, a variety of nonlinear effects such as harmonic generation and all optical modulation can be enabled and enhanced at the nanoscale. This review presents our research on engineering and boosting nonlinear effects in ultrafast and nonlinear semiconductor metasurfaces fabricated at the Center for Integrated Nanotechnologies (CINT). We cover our recent works on parametric generation of harmonic light via direct and cascade…
We present an ultrafast all-optical gated amplifier, or transistor, consisting of a forest of ZnO nanowire lasers. A gate light pulse creates a dense electron-hole plasma and excites laser action inside the nanowires. Source light traversing the nanolaser forest is amplified, partly as it is guided through the nanowires, and partly as it propagates diffusively through the forest. We have measured transmission increases at the drain up to a factor 34 for 385-nm light. Time-resolved amplification measurements show that the lasing is rapidly self-quenching, yielding pulse responses as short as 1.…
We demonstrate ultrafast dephasing in the random transport of light through a layer consisting of strongly scattering GaP nanowires. Dephasing results in a nonlinear intensity modulation of individual pseudomodes which is 100 times larger than that of bulk GaP. Different contributions to the nonlinear response are separated using total transmission, white-light frequency correlation, and statistical pseudomode analysis. A dephasing time of $1.2\pm 0.2$~ps is found. Quantitative agreement is obtained with numerical model calculations which include photoinduced absorption and deformation of indi…
Hybrid nanocomposites can offer a wide range of opportunities to control the light-matter interac- tion and electromagnetic energy flow at the nanoscale, leading to exotic optoelectronic devices. We study theoretically the dipole-dipole interaction in noble metal nanoparticles-graphene nanodisks- quantum dots hybrid systems in the optical region of the electromagnetic spectrum. The quantum dot is assumed to be a three-level atom interacting with ultrashort control and probe pulses in a Lambda configuration. The dynamics of the system are studied by numerically solving for the time evo- lution …
The future interconnect links in intra- and inter-chip require the photodetector with high bandwidth, ultra-wide waveband, compact footprint, low-cost, and compatible integration process with silicon complementary metal-oxide-semiconductor (CMOS) technology. Here, we demonstrate a CMOS-compatible carbon nanotube (CNT) photodetector that exhibits high responsivity, high bandwidth and broad spectral operation over all optical telecommunication band based on high-purity CNT arrays. The ultrafast CNT photodetector demonstrates the 100 Gbit/s Nyquist-shaped on-off-keying (OOK) signal transmission, …
We demonstrate a new concept for reconfigurable nanophotonic devices exploiting ultrafast nonlinear control of shaped wavefronts in a multimode nanomaterial consisting of semiconductor nanowires. Femtosecond pulsed laser excitation of the nanowire mat is shown to provide an efficient nonlinear mechanism to control both destructive and constructive interference in a shaped wavefront. Modulations of up to 63% are induced by optical pumping, due to a combination of multimode dephasing and induced transient absorption. We show that part of the nonlinear phase dynamics can be inverted to provide a …
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…
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 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…
The quest to improve density, speed and energy efficiency of magnetic memory storage has led to exploration of new ways of optically manipulating magnetism at the ultrafast time scale, in particular in ferrimagnetic alloys. While all-optical magnetization switching is well-established on the femtosecond timescale, lateral nanoscale confinement and thus potential significant reduction of the size of the magnetic element remains an outstanding challenge. Here we employ resonant electromagnetic energy-funneling plasmon nanoantennas to influence the demagnetization dynamics of a ferrimagnetic TbCo…
We have demonstrated for the first time that an array of nanoantennas (central nanotips inside sub-micron pits) on an aluminum surface, fabricated using a specific double-pulse femtosecond laser irradiation scheme, results in a 28-fold enhancement of the non-linear (three-photon) electron photoemission yield, driven by a third intense IR femtosecond laser pulse. The supporting numerical electrodynamic modeling indicates that the electron emission is increased not owing to a larger effective aluminum surface, but due to instant local electromagnetic field enhancement near the nanoantenna, contr…
The coherence of polaritons plays a fundamental role in numerous recent experimental observations, from strong coupling to Bose-Einstein condensation, but accessing the coherence of polaritons is a difficult task due to the high energy of plasmons and excitons. However, surface phonon polaritons offer similar promises at much lower energy. Here, we demonstrate the possibility to use visible ultrafast lasers to generate and time resolve coherent surface phonon polaritons in nanowires. We show that these modes are generated through the ultrafast screening of the surface depletion field. By compa…
Dynamical materials that capable of responding to optical stimuli have always been pursued for designing novel photonic devices and functionalities, of which the response speed and amplitude as well as integration adaptability and energy effectiveness are especially critical. Here we show ultrafast pulse generation by exploiting the ultrafast and sensitive nonlinear dynamical processes in tunably solution-processed colloidal epsilon-near-zero (ENZ) transparent conducting oxide (TCO) nanocrystals (NCs), of which the potential respond response speed is >2 THz and modulation depth is ~23% pumped …
Ultrafast laser pulses spatially shaped as Bessel beams in dielectrics create high aspect ratio plasma channels whose relaxation can lead to the formation of nanochannels. We report a strong enhancement of the nanochannel drilling efficiency with illumination by double pulses separated by a delay between 10 to 500 ps. This enables the formation of nanochannels with diameters down to 100 nm. Experimental absorption measurements demonstrate that the increase of drilling efficiency is due to an increase of the confinement of the energy deposition. Nanochannel formation corresponds to a drastic ch…
We demonstrate ultrafast soliton-based nonlinear balancing of dual-core asymmetry in highly nonlinear photonic crystal fiber at sub-nanojoule pulse energy level. The effect of fiber asymmetry was studied experimentally by selective excitation and monitoring of individual fiber cores at different wavelengths between 1500 nm and 1800 nm. Higher energy transfer rate to non-excited core was observed in the case of fast core excitation due to nonlinear asymmetry balancing of temporal solitons, which was confirmed by the dedicated numerical simulations based on the coupled generalized nonlinear Schr…
Ultrafast Nano-Imaging and Optical Control of Hyperbolic Phonon Polaritons at hBN/WS$_2$ Heterojunctions
Institute for Molecular Science, National Institutes of Natural Sciences（国立自然科学研究所分子科学研究所）；Department of Physics and Electronics, Graduate School of Engineering, Osaka Metropolitan University（大阪公立大学工学研究科物理电子学专业）；The Graduate University for Advanced Studies, SOKENDAI（日本高级研究院）；Research Center for Materials Nanoarchitectonics, National Institute for Materials Science（国立材料研究所物质结构纳米构造研究中心）；Research Center for Electronic and Optical Materials, National Institute for Materials Science（国立材料研究所电子光学材料研究中心）；Fritz-Haber-Institut der Max-Planck-Gesellschaft（马克斯·普朗克学会弗里茨·哈伯研究所）
In recent years, the computational demands of deep learning applications have necessitated the introduction of energy-efficient hardware accelerators. Optical neural networks are a promising option; however, thus far they have been largely limited by the lack of energy-efficient nonlinear optical functions. Here, we experimentally demonstrate an all-optical Rectified Linear Unit (ReLU), which is the most widely used nonlinear activation function for deep learning, using a periodically-poled thin-film lithium niobate nanophotonic waveguide and achieve ultra-low energies in the regime of femtojo…
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…
Light-induced magnetization changes, such as all-optical switching, skyrmion nucleation, and intersite spin transfer, unfold on temporal and spatial scales down to femtoseconds and nanometers, respectively. Pump-probe spectroscopy and diffraction studies indicate that spatio-temporal dynamics may drastically affect the non-equilibrium magnetic evolution. Yet, direct real-space magnetic imaging on the relevant timescale has remained challenging. Here, we demonstrate ultrafast high-harmonic nanoscopy employing circularly polarized high-harmonic radiation for real-space imaging of femtosecond mag…
By using femtosecond laser pulses at a wavelength range from 720 to 780 nm, we have observed absorptive and refractive nonlinearities in a film of multi-walled carbon nanotubes grown mainly along the direction perpendicular to the surface of quartz substrate. The Z-scans show that both absorptive and refractive nonlinearities are of negative and cubic nature in the laser irradiance range from a few to 300 GW/cm^2. The magnitude of the third-order nonlinear susceptibility,chi-(3), is of an order of 10^-11 esu. The degenerate pump-probe measurement reveals a relaxation time of 2 ps.
