Laser-induced modification of transparent solids by intense femtosecond laser pulses allows fast integration of nanophotonic and nanofluidic devices with controlled optical properties. So far, the local and dynamic nature of the interactions between plasma and light needed to correctly explain nanograting fabrication on dielectric surfaces has been missing in the theoretical models. With our numerical approach, we show that a self-consistent dynamic treatment of the plasma formation and its interaction with light triggers an ultrafast reconfiguration of the periodic plasma patterns on a field-cycle time scale. Within this framework, a simple stability analysis of the local interactions explains how the laser-induced plasma patterns change their orientation with respect to the incident light polarization, when a certain energy density threshold is reached. Moreover, the reconfigured sub-wavelength plasma structures grow into the bulk of the sample and agree with the experimental findings of self-organized volume nanogratings. Mode coupling of the incident and transversally scattered light with the periodic plasma structures is sufficient to initiate the growth and the self-organization of the characteristic pattern with a periodicity of a half-wavelength in the medium.
We propose to use femtosecond direct laser writing technique to realize dielectric optical elements from photo-resist materials for the generation of structured light from purely geometrical phase transformations. This is illustrated by the fabrication and characterization of spin-to-orbital optical angular momentum couplers generating optical vortices of topological charge from 1 to 20. In addition, the technique is scalable and allows obtaining microscopic to macroscopic flat optics. These results thus demonstrate that direct 3D photopolymerization technology qualifies for the realization of…
We investigate the interaction of trains of femtosecond microjoule laser pulses with dielectric materials by means of a multi-scale model. Our theoretical predictions are directly confronted with experimental observations in soda-lime glass. We show that due to the low heat conductivity, a significant fraction of the laser energy can be accumulated in the absorption region. Depending on the pulse repetition rate, the material can be heated to high temperatures even though the single pulse energy is too low to induce a significant material modification. Regions heated above the glass transition…
The mechanism of ablation of solids by intense femtosecond laser pulses is described in an explicit analytical form. It is shown that at high intensities when the ionization of the target material is complete before the end of the pulse, the ablation mechanism is the same for both metals and dielectrics. The physics of this new ablation regime involves ion acceleration in the electrostatic field caused by charge separation created by energetic electrons escaping from the target. The formulae for ablation thresholds and ablation rates for metals and dielectrics, combining the laser and target p…
The formation of an electron-hole plasma during the interaction of intense femtosecond laser pulses with transparent solids lies at the heart of femtosecond laser processing. Advanced micro- and nanomachining applications require improved control over the excitation characteristics. Here, we relate the emission of low-order harmonics to the strong laser-field-induced plasma formation. Together with a measurement of the total plasma density we identify the contribution of two competing ionization mechanisms - strong-field and electron-impact ionization.
Electromagnetic radiation within the terahertz (THz) frequency range is of great interest for applications in remote sensing and time-domain spectroscopy. The laser-induced plasmas are promising mediums for generating THz radiation. It has been recently reported that focusing femtosecond Bessel pulses inside dielectrics induces a high aspect ratio over-critical plasmas. Here we show that the intense resonantly driven electrostatic fields at the so-called critical surface lead to THz radiation emission. Through three-dimensional particle-in-cell simulation and analytical derivation, we have inv…
Optical metasurfaces have come into the spotlight as a promising platform for light manipulation at the nanoscale, including ultrafast all-optical control via excitation with femtosecond laser pulses. Recently, dichroic metasurfaces have been exploited to modulate the polarization state of light with unprecedented speed. Here, we theoretically predict and experimentally demonstrate by pump-probe spectroscopy the capability to reconfigure the ultrafast dichroic signal of a gold metasurface by simply acting on the polarization of the pump pulse, which is shown to reshape the spatio-temporal dist…
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…
Second-harmonic emission at a frequency that is twice the laser frequency is an important diagnostic for nonlinear laser-plasma interaction. It is forbidden for centrosymmetric materials such as the bulk of sapphire. The symmetry, however, can be broken by dielectric discontinuities as a result of plasma generation inside a solid dielectric. In the present work, we explore the basic characteristics of experimentally observed second-harmonic emission during focusing a femtosecond Bessel beam inside sapphire. We employ three-dimensional particle-in-cell simulations and the Helmholtz wave equatio…
We theoretically investigate the dynamical Franz-Keldysh effect in femtosecond time resolution, that is, the time-dependent modulation of a dielectric function at around the band gap under an irradiation of an intense laser field. We develop a pump-probe formalism in two distinct approaches: first-principles simulation based on real-time time-dependent density functional theory and analytic consideration of a simple two-band model. We find that, while time-average modulation may be reasonably described by the static Franz-Keldysh theory, a remarkable phase shift is found to appear between the …
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
Experimental and theoretical studies of laser-induced breakdown in dielectrics provide conflicting conclusions about the possibility to trigger ionization avalanche on the sub-picosecond time scale and the relative importance of carrier-impact ionization over field ionization. On the one hand, current models based on single ionization-rate equations do not account for the gradual heating of the charge carriers which, for short laser pulses, might not be sufficient to start an avalanche. On the other hand, models based on multiple rate equations that track the carriers kinetics rely on several …
We report on fabrication of whispering-gallery-mode microlasers in a Nd:glass chip by femtosecond laser three-dimensional (3D) micromachining. Main fabrication procedures include the fabrication of freestanding microdisks supported by thin pillars by femtosecond laser ablation of the glass substrate immersed in water, followed by CO2 laser annealing for surface smoothing. Lasing is observed at a pump threshold as low as ~69 μW at room temperature with a continuous-wave laser diode operating at 780nm. This technique allows for fabrication of microcavities of high quality factors in various diel…
We report three-dimensional laser microfabrication, which enables microstructuring of materials on the scale of 0.2-1 micrometers. The two different types of microfabrication demonstrated and discussed in this work are based on holographic recording, and light-induced damage in transparent dielectric materials. Both techniques use nonlinear optical excitation of materials by ultrashort laser pulses (duration < 1 ps).
Ultrafast, femtosecond laser pulse interaction with dielectric materials has shown them to have significantly higher laser fluence threshold requirements, as compared to metals and semiconductors, for laser material modification, such as laser ablation. Examples of dielectrics are crystalline materials such as quartz and sapphire, and amorphous glasses. The interaction between femtosecond laser pulses, at a wavelength with negligible linear absorption, and a dielectric has been found to be weak, and multiple pulse irradiation is therefore typically used in order to see significant and quantifi…
We quantify the dependence of the single-shot ablation threshold on the angle of incidence and polarization of a femtosecond laser beam, for three dissimilar solid-state materials: a metal, a dielectric and a semiconductor. Using the constant, linear value of the index of refraction, we calculate the laser fluence transmitted through the air-material interface at the point of ablation threshold. We show that, in spite of the highly nonlinear ionization dynamics involved in the ablation process, the so defined transmitted threshold fluence is universally independent of the angle of incidence an…
Inspired by the ever-increasing demand for higher data transmission rates and the tremendous attention toward all-optical signal processing based on miniaturized nanophotonics, in this paper, for the first time, we investigate the integrable design of coherent ultrashort light pulse code-division multiple-access (CDMA) technique, also known as femtosecond CDMA, using all-dielectric metasurfaces (MSs). In this technique, the data bits are firstly modulated using ultrashort femtosecond optical pulses generated by mode-locked lasers, and then by employing a unique phase metamask for each data str…
The creation of high energy density ($\gtrsim10^6$ joules per cm$^3$) over-critical plasmas in a large volume has essential applications in the study of warm dense matter, being present in the hot cores of stars and planets. It was recently shown that femtosecond Bessel beams enable creating over-critical plasmas inside sapphire with sub-wavelength radius and several tens of micrometers in length. Here, the dependence of field structure and absorption mechanism on the plasma density transverse profile are investigated by performing self-consistent Particle-In-Cell (PIC) simulations. Two { limi…
In-line Dispersion Control of Femtosecond Laser Pulses by Multilayer Huygens' Metasurfaces
Friedrich-Schiller-University Jena（耶拿弗里德里希·席勒大学）；Australian National University（澳大利亚国立大学）；Fraunhofer Institute for Applied Optics and Precision Engineering IOF（弗劳恩霍夫应用光学和精密工程研究所）
We demonstrate for the first time to our knowledge the generation of overcritical plasma densities inside transparent solids over long distances using femtosecond laser pulses. This opens new avenues for high energy density physics in confined geometry such as warm dense matter study or the synthesis of new material phases. We show both with experiments and first-principles simulations, that femtosecond conical interference via a Bessel beam creates a dense plasma rod with typically 100 nm diameter in sapphire. The interaction is in ideal conditions to trigger collisionless resonance absorptio…
Laser-induced plasma formation and subsequent relaxation in solid dielectrics is the precursor to structural modifications that are accompanied by a permanent alteration of material properties. The decay of the electron-hole plasma through distinct relaxation channels determines the properties of the resulting modification. Based on an experimental arrangement combining a time-resolved transmission measurement with a cross-phase modulation measurement, we isolate the plasma formation and relaxation dynamics in the bulk of amorphous fused silica excited by femtosecond short-wavelength infrared …
Tunable coherent light sources operating in the vacuum ultraviolet (VUV) region in 100-200-nm (6-12 eV) wavelength range have important spectroscopic applications in many research fields, including time-resolved angle-resolved photoemission spectroscopy (ARPES). Recent advances in laser technology have enabled the upconversion of visible femtosecond lasers to the vacuum and extreme ultraviolet regions. However, the complexity of their experimental setups and the scarcity of bulk nonlinear crystals for VUV generation have hampered its widespread use. Here, we propose the use of a free-standing …
A wavelength-degenerate pump-probe spectroscopy is used to study the ultrafast dynamics of strong-field ionization in femtosecond-laser subwavelength-structured fused silica. The comparative spectra demonstrate that femtosecond-laser subwavelength structuring always give rise to great enhancement for strong-field ionization as well as third-order nonlinear optical effects, which is the direct evidence of great local field enhancement in subwavelength apertures of fs-laser highly-excited surface. In short, the study shows the prominent subwavelength spatial effect of strong-field ionization in …
In recent years resonant semiconductor and all-dielectric nanophotonics offered a lot of possibilities for thermally-induced light manipulation at the nanoscale. Owing to high-quality resonant states, such nanostructures allow for efficient light-to-heat conversion supported by various temperature detection approaches based on thermally sensitive intrinsic optical responses (photoluminescence, Raman scattering, thermorefraction etc.). In this work, we study theoretically a phenomenon of the photothermal reshaping of the radiation pattern of second-harmonic generation (SHG) that occurs in reson…
The reversible phase transition induced by femtosecond laser excitation of Gallium has been studied by measuring the dielectric function at 775 nm with ~ 200 fs temporal resolution. The real and imaginary parts of the transient dielectric function were calculated from absolute reflectivity of Gallium layer measured at two different angles of incidence, using Fresnel formulas. The time-dependent electron-phonon effective collision frequency, the heat conduction coefficient and the volume fraction of a new phase were restored directly from the experimental data, and the time and space dependent …
The electron dynamics in dielectric materials induced by intense femtosecond laser pulses is theoretically addressed. The laser driven temporal evolution of the energy distribution of electrons in the conduction band is described by a kinetic Boltzmann equation. In addition to the collisional processes for energy transfer such as electron-phonon-photon and electron-electron interactions, a non-collisional process for photon absorption in the conduction band is included. It relies on direct transitions between sub-bands of the conduction band through multiphoton absorption. This mechanism is sh…
We report the appearance of transient Newton rings in dielectrics (sapphire and lead-oxide glass) during ablation with single fs laser pulses. Employing femtosecond microscopy with 800 nm excitation and 400 nm illumination, we observe a characteristic ring pattern that dynamically changes for increasing delay times between pump and probe pulse. Such transient Newton rings have been previously observed in metals and semiconductors at fluences above the ablation threshold and were related to optical interference of the probe beam reflected at the front surface of the ablating layer and at the in…
Laser filamentation in transparent material has a wide range of applications, from three dimensional manufacturing to biological technologies. Various experimental results showed that femtosecond laser pulse filamentation in fused silica strongly depends on laser focusing conditions. However, the physical mechanism governing each regime has not been fully understood. For the first time, single and multiple re-focusing of the laser pulse in interaction of femtosecond laser pulse with fused silica, and consequent single and multiple damage zones (filaments) have been observed in our extensive th…
We describe a high-speed single-shot multi-frame interferometric imaging technique enabling multiple interferometric images with femtosecond exposure time over a 50 ns event window to be recorded following a single laser-induced excitation event. The stroboscopic illumination of a framing camera is made possible through the use of a doubling cavity which produces a femtosecond pulse train that is synchronized to the gated exposure windows of the individual frames of the camera. The imaging system utilizes a Michelson interferometer to extract phase and ultimately displacement information. We d…
Currently, direct-write waveguide fabrication is probably the most widely studied application of femtosecond laser micromachining in transparent dielectrics. Devices such as buried waveguides, power splitters, couplers, gratings and optical amplifiers have all been demonstrated. Waveguide properties depend critically on the sample material properties and writing laser characteristics. In this paper we discuss the challenges facing researchers using the femtosecond laser direct-write technique with specific emphasis being placed on the suitability of fused silica and phosphate glass as device h…
The non-linear response of dielectrics to intense, ultrashort electric fields has been a sustained topic of interest for decades with one of its most important applications being femtosecond laser micro/nano-machining. More recently, renewed interests in strong field physics of solids were raised with the advent of mid-infrared femtosecond laser pulses, such as high-order harmonic generation, optical-field-induced currents, etc. All these processes are underpinned by photoionization (PI), namely the electron transfer from the valence to the conduction bands, on a time scale too short for phono…
We theoretically investigate the generation of ultrafast currents in insulators induced by strong few-cycle laser pulses. Ab initio simulations based on time-dependent density functional theory give insight into the atomic-scale properties of the induced current signifying a femtosecond-scale insulator-metal transition. We observe the transition from nonlinear polarization currents during the laser pulse at low intensities to tunnelinglike excitation into the conduction band at higher laser intensities. At high intensities, the current persists after the conclusion of the laser pulse considere…
Controlling and confining light by exciting plasmons in resonant metallic nanostructures is an essential aspect of many new emerging optical technologies. Here we explore the possibility of controllably reconfiguring the intrinsic optical properties of semi-continuous gold films, by inducing permanent morphological changes with a femtosecond (fs)-pulsed laser above a critical power. Optical transmission spectroscopy measurements show a correlation between the spectra of the morphologically modified films and the wavelength, polarization, and the intensity of the laser used for alteration. In o…
The concept of high refractive index subwavelength dielectric nanoresonators, supporting electric and magnetic optical resonances, is a promising platform for waveguiding, sensing, and nonlinear nanophotonic devices. However, high concentration of defects in the nanoresonators diminishes their resonant properties, which are crucially dependent on their internal losses. Therefore, it seems to be inevitable to use initially crystalline materials for fabrication of the nanoresonators. Here, we show that the fabrication of crystalline (low-loss) resonant silicon nanoparticles by femtosecond laser …
Nonlinear Self-Action across Temporal Regimes in Resonant Dielectric Metasurfaces
Politecnico di Milano（米兰理工大学）；Institute of Photonic and Nanotechnology (IFN) - Consiglio Nazionale delle Ricerche (CNR)（光子与纳米技术研究所（IFN）- 意大利国家研究委员会（CNR））；Institute of Photonics and Quantum Sciences, Heriot-Watt University（赫瑞-瓦特大学光子与量子科学研究所）；ICFO - Institut de Ciències Fotòniques, the Barcelona Institute of Science and Technology（ICFO - 巴塞罗那科学和技术理工学院光子科学研究所）；Università degli Studi di Brescia（布雷西亚大学）
We have developed low-dispersion (1480 l/mm), resonance-free, diffraction gratings made of dielectric materials resistant to femtosecond laser damage $(SiO_{2}/HfO_{2})$. A 14 cm diameter sample was fabricated resulting in a mean diffraction efficiency of 99.1% at λ = 810 nm with 0.4% uniformity using equipment which can fabricate gratings up to 1m diagonal. The implementation of these gratings in the compression of 30 fs pulses in an out-of-plane geometry can result in compressor efficiencies of ~95%. The measured laser absorption is 500x lower than current ultrafast petawatt-class compressor…
Various clusters of metallic or dielectric nanoparticles can exhibit sharp Fano resonances originating from at least two modes interference of different spectral width. However, for practical applications such as biosensing or nonlinear nanophotonics, the fine-tuning of the Fano resonances is generally required. Here, we propose and demonstrate a novel type of hybrid oligomers consisting of asymmetric metal-dielectric (Au/Si) nanoparticles with a sharp Fano resonance in visible range, which has a predominantly magnetic origin. We demonstrate both, numerically and experimentally, that such hybr…
Dielectric laser acceleration is a versatile scheme to accelerate and control electrons with the help of femtosecond laser pulses in nanophotonic structures. We demonstrate here the generation of a train of electron pulses with individual pulse durations as short as $270\pm80$ attoseconds(FWHM), measured in an indirect fashion, based on two subsequent dielectric laser interaction regions connected by a free-space electron drift section, all on a single photonic chip. In the first interaction region (the modulator), an energy modulation is imprinted on the electron pulse. During free propagatio…
Asymmetric metal-dielectric nanostructures are demonstrated superior optical properties arise from the combination of strong enhancement of their near fields and controllable scattering characteristics which originate from plasmonic and high-index dielectric components. Here, being inspired by the recent experimental work [Dmitry~Zuev, \textit{et al.}, Adv. Mater. \textbf{28}, 3087 (2016)] on a new technique for fabrication of asymmetric hybrid nanoparticles via femtosecond laser melting at the nanoscale, we suggest and study numerically a novel type of hybrid dimer nanoantennas. The nanoanten…
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…
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…
We show that recently observed DC currents produced by below-the-bandgap femtosecond pulses [1] can be explained as nonlinear optical effects based on multi-photon quantum interference and creation of an asymmetric distribution of virtual carriers in the conduction and valence bands. We establish an unambiguous connection between the nonlinear optical conductivity responsible for the observed DC currents and charges and the odd-order nonlinear optical susceptibilities of the material. Using a single well known measured value of the third order susceptibility (nonlinear index) of SiO2 we obtain…
We report enhanced broadband Terahertz (THz) generation and detailed characterization from the interaction of femtosecond two colour laser pulses with thin transparent dielectric tape target in ambient air. The proposed source is easy to implement, exhibits excellent scalability with laser energy. Spectral characterization using Fourier transform spectrometer reveals yield enhancement of more than 150 % in the THz region of 0.1 - 10 THz with respect to conventional two-colour laser plasma source in ambient air. Further, the source spectrum extends up to 40 THz with an enhancement of flux > 30 …
A femtosecond laser pulse is able to switch the magnetic state of a 3d-4f ferrimagnetic material on a pico-second time scale. Devices based on this all-optical switching (AOS) mechanism are competitive candidates for ultrafast memory applications. However, a large portion of the light energy is lost by reflection from the metal thin film as well as transmission to the substrate. In this paper, we explore the use of dielectric coatings to increase the light absorption by the magnetic metal layer based on the principle of constructive interference. We experimentally show that the switching energ…
The employment of ultrashort laser sources at the mid-IR spectral region for transparent materials is designed to open new routes for laser patterning and a wealth of exciting applications in optics and photonics. To elucidate the material response to irradiation with mid-IR laser sources, a consistent analysis of the interaction of long wavelength femtosecond pulses with dielectric materials is presented. The influence of the pulse duration is, in particularly, emphasized towards specifying the laser parameters for which photoionization and impact ionization are important. Simulations results…
A computer simulation of dynamics of an optical discharge produced in the volume of a transparent dielectric (fused silica) by a focused femtosecond laser pulse was carried out taking into account the possibility of developing small-scale ionization-field instability. The presence of small foreign inclusions in the fused silica was taken into account with the model of a nanodispersed heterogeneous medium by using Maxwell Garnett formulas. The results of the calculations made it possible to reveal the previously unknown physical mechanism that determines the periodicity of the ordered plasma-fi…
Exposure of metal surfaces to multiple ultrashort laser pulses under certain conditions leads to the formation of well-defined periodic surface structures. We show how the period of such structures in steel can be tuned over a wide range by controlling the complex interaction mechanisms triggered in the material. Amongst the different irradiation parameters that influence the properties of the induced structures, the angle of incidence of the laser beam occupies a prominent role. We present an experimental and theoretical investigation of this angle dependence in steel upon irradiation with la…
A comparative study is performed to explore the periodic structure formation upon intense femtosecond pulsed irradiation of dielectrics with radially and azimuthally polarised beams. Laser conditions have been selected appropriately to produce excited carriers with densities below the optical breakdown threshold in order to highlight the role of phase transitions in surface modification mechanisms. The frequency of the laser induced structures is calculated based on a theoretical model that comprises estimation of electron density excitation, heat transfer, relaxation processes, and hydrodynam…
Tunable supercontinuum in multimode fiber via bending-induced dispersion modification
Massachusetts Institute of Technology（麻省理工学院）；Research Laboratory of Electronics, Massachusetts Institute of Technology（麻省理工学院电子研究实验室）；Department of Biology, Massachusetts Institute of Technology（麻省理工学院生物学系）；Beth Israel Deaconess Medical Center, Harvard Medical School（哈佛医学院贝斯以色列女执事医疗中心）
A systematic analysis of polarization effects in a direct write femtosecond laser 3D lithography is presented. It is newly shown that coupling between linear polarization of the writing light electric field and temperature gradient can be used to fine-tune feature sizes in structuring of photoresists at a nanoscale. The vectorial Debye focusing is used to simulate polarization effects and a controlled variation up to 20% in the linewidth is shown experimentally for the identical axial extent of the polymerised features. The revealed mechanisms are relevant for a wide range of phenomena of ligh…
Ultrafast electron dynamics in solids under strong optical fields has recently found particular attention. In dielectrics and semiconductors, various light-field-driven effects have been explored, such as high-harmonic generation, sub-optical-cycle interband population transfer and nonperturbative increase of transient polarizability. In contrast, much less is known about field-driven electron dynamics in metals because charge carriers screen an external electric field in ordinary metals. Here we show that atomically thin monolayer Graphene offers unique opportunities to study light-field-driv…
