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 parameters, are derived and compared to experimental data. The calculated dependence of the ablation thresholds on the pulse duration is in agreement with the experimental data in a femtosecond range, and it is linked to the dependence for nanosecond pulses.
We investigated femtosecond laser ablation dynamics using THz time-domain spectroscopy. To clarify the breakdown dynamics of materials, we focused on the motion of charged particles and measured the terahertz waves emitted during laser ablation. We revealed that the Coulomb force dominated the ablation process. Furthermore, comparisons of the experimental results with theoretical models showed that material breakdown occurs within a few hundred femtoseconds. Our experimental results indicate that electrostatic ablation is the most likely ablation mechanism for metals.
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…
In femtosecond laser micromachining, the ablation threshold is a key processing parameter that characterises the energy density required to cause ablation. Current techniques for measuring the ablation threshold such as the diameter regression and diagonal scan methods are based on the assumption of a Gaussian spatial profile, however no techniques currently exist for measuring the ablation threshold using a non-Gaussian beam shape. Here we present a formalism of the diagonal scan method for determining the ablation threshold and pulse superposition for femtosecond vortex pulses. To the author…
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…
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…
Fast fabrication of micro-optical elements for generation of optical vortex beams based on the q-plate design is demonstrated by femtosecond (fs) laser ablation of gold film on glass. Q-plates with diameter of ~0.5 mm were made in ~1 min using galvanometric scanners with writing speed of 5 mm/s. Period of gratings of 0.8 micrometers and groove width of 250 nm were achieved using fs-laser ablation at 343 nm wavelength. Phase and intensity analysis of optical vortex generators was carried out at 633 nm wavelength and confirmed the designed performance. Efficiency of spin-orbital conversion of th…
Femtosecond-to-millisecond holographic imaging of laser ablation dynamics
Institute for Photon Science and Technology, The University of Tokyo（光子科学技术研究所，东京大学）；Department of Advanced Materials Science, The University of Tokyo（先进材料科学系，东京大学）；RIKEN Center for Advanced Photonics, RIKEN（理化学研究所先进光子学中心，理化学研究所）
Femtosecond laser ablation of Ti, Zr and Hf has been investigated by means of in-situ plasma diagnostics. Fast plasma imaging with the aid of an intensified charged coupled device (ICCD) camera was used to characterise the plasma plume expansion on a nanosecond time scale. Time- and spaceresolved optical emission spectroscopy was employed to perform time-of-flight measurements of ions and neutral atoms. It is shown that two plasma components with different expansion velocities are generated by the ultra-short laser ablation process. The expansion behaviour of these two components has been anal…
We demonstrate that thousands of periodic nano-craters are fabricated on a subwavelength-diameter tapered optical fiber, an optical nanofiber, by irradiating with just a single femtosecond laser pulse. A key aspect of the fabrication is that the nanofiber itself acts as a cylindrical lens and focuses the femtosecond laser beam on its shadow surface. We also demonstrate that such periodic structures on the nanofiber, act as a 1-D photonic crystal (PhC). Such PhC structures on the nanofiber will strongly enhance the field confinement in such a tapered fiber-based system and may open new avenues …
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…
We report the physical reasons of a curious decrease in the crater depth observed for long delays in experiments with femtosecond double pulses. Detailed hydrodynamic modeling demonstrates that the ablation mechanism is dumped when the delay between the pulses exceeds the electron-ion relaxation time. In this case, the interaction of the second laser pulse with the expanding target material leads to the formation of the second shock wave suppressing the rarefaction wave created by the first pulse. The evidence of this effect follows from the pressure and density profiles obtained at different …
Laser direct writing is an attractive method for patterning 2D materials without contamination. Literature shows that the femtosecond ablation threshold of graphene across substrates varies by an order of magnitude. Some attribute it to the thermal coupling to the substrates, but it remains by and large an open question. For the first time the effect of substrates on femtosecond ablation of 2D materials is studied using MoS$_{2}$ as an example. We show unambiguously that femtosecond ablation of MoS$_{2}$ is an adiabatic process with negligible heat transfer to the substrates. The observed thre…
We experimentally demonstrate the use of subwavelength optical nanoantennae to assist the gentle ablation of nanostructures directly using ultralow fluence from a Ti: sapphire oscillator through the excitation of surface plasmon waves. We show that this ablation mechanism is the same for metal and dielectric. The analytical solutions of ablation threshold are in excellent agreement with the experiment estimations. Surface plasmon assisted locally enhanced ablation at nanoscale provides a method for nanomachining, manipulation and modification the nanostructures without collateral thermal damag…
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…
Femtosecond micromachining offers a contact-free and mask-less technique for material patterning. With ultrafast laser irradiation, permanent modifications to the properties of single layer graphene through material ablation or defect introduction can be induced. Multiple femtosecond pulse interactions with a single layer graphene are studied and a low laser ablation threshold ~9.2 mJ/cm2 is reported for a 15 second illumination time. Clean ablated structures are generated in such a multi pulse irradiation configuration at low pulse energies as an attractive alternative to ablation with single…
In this work, for the first time of our knowledge, we present a well-supported procedure to fabricate ridge optical waveguides onto thin films of PLZT by femtosecond laser ablation. In order to achieve smooth guiding structures to guarantee good optical performance, we have studied the ablation threshold characteristics for different kinematic conditions of fs laser machining and also we have explored the different ablation regimens for several fluencies reached. Besides, we characterize the morphology and roughness of ridge waveguides through a modal and scattering loss analysis, for waveguid…
Femtosecond pulses hold great promise for high-precision tissue removal. However, ablation rates are severely limited by the need to keep average laser power low to avoid collateral damage due to heat accumulation. Furthermore, previously reported pulse energies preclude delivery in flexible fibers, hindering in vivo operation. Both of these problems can be addressed through use of groups of high-repetition-rate pulses, or bursts. Here, we report a novel fiber laser and demonstrate ultrafast burst-mode ablation of brain tissue at rates approaching 1 mm$^3$/min, an order of magnitude improvemen…
We report on the experimental observation of selective delamination of semi-transparent materials on the example of yttria-stabilized zirconia ceramics upon femtosecond laser processing of its surface with low numerical aperture lens. The delamination of a ceramic layer of dozens of micrometers takes place as a by-side effect of surface processing and is observed above the surface ablation threshold. The onset of delamination (delamination threshold) depends on the degree of overlap of the irradiation spots from consecutive laser pulses upon beam scanning over material surface. Analysis of the…
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-…
Fabrication of large area (sub 1 cm cross-section) micro-optical components in a short period of time (approximately 10 min) and with lesser number of processing steps is highly desirable and cost-effective. In the recent years, femtosecond laser fabrication technology has revolutionized the field of manufacturing by offering the above capabilities. In this study, a fundamental diffractive optical element, binary axicon i.e axicon with two phase or amplitude levels, has been designed in three configurations namely conventional axicon, photon sieve axicon (PSA) and sparse PSA and directly mille…
We propose a feedback-assisted direct laser writing method to perform laser ablation of fiber optics devices in which their light-collection signal is used to optimize their properties. A femtosecond-pulsed laser beam is used to ablate a metal coating deposited around a tapered optical fiber, employed to show the suitability of the approach to pattern devices with small radius of curvature. During processing, the same pulses generate two-photon fluorescence in the surrounding environment and the signal is monitored to identify different patterning regimes over time through spectral analysis. T…
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…
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…
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…
Hybrid Femtosecond Laser and Ion-Implantation Processing for Controlled, Deep, High-Efficiency Ablation in Fused Silica
Instituto de Optica Daza de Valdes (IO), CSIC（西班牙科学研究中心光学研究所）；HiLASE Centre, FZU - Institute of Physics of the Czech Academy of Sciences（捷克科学院物理研究所 HiLASE 中心）；Universidad Autónoma de Madrid（马德里自治大学）；Centro de Microanálisis de Materiales (CMAM), Universidad Autónoma de Madrid（马德里自治大学材料微分析中心）；FZU - Institute of Physics of the Czech Academy of Sciences（捷克科学院物理研究所）
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…
Although ultrafast laser materials processing has advanced at a breakneck pace over the last two decades, most applications have been developed with laser pulses at near-IR or visible wavelengths. Recent progress in mid-infrared (MIR) femtosecond laser source development may create novel capabilities for material processing. This is because, at high intensities required for such processing, wavelength tuning to longer wavelengths opens the pathway to a special regime of laser-solid interactions. Under these conditions, due to the $λ^2$ scaling, the ponderomotive energy of laser-driven electron…
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.
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 …
Short laser pulse in wide range of wavelengths, from infrared to X-ray, disturbs electron-ion equilibrium and rises pressure in a heated layer. The case where pulse duration $τ_L$ is shorter than acoustic relaxation time $t_s$ is considered in the paper. It is shown that this short pulse may cause thermomechanical phenomena such as spallative ablation regardless to wavelength. While the physics of electron-ion relaxation on wavelength and various electron spectra of substances: there are spectra with an energy gap in semiconductors and dielectrics opposed to gapless continuous spectra in metal…
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 report that femtosecond surface plasmon polariton pulses can propagate along a metal-dielectric waveguide and that they can be modulated on the femtosecond timescale by direct ultrafast optical excitation of the metal, thereby offering unprecedented terahertz plasmonic bandwidth - a key missing component in the development of surface plasmons as information carriers for next generation nanophotonic devices.
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 …
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…
Electronic devices are progressively fabricated on flexible substrates allowing new fields of applications. A maskless and very flexible structuring process is offered by ablation using ultra-short pulse laser irradiation. Usually, certain areas of a functional thin film coating are locally removed to yield the needed device structures. Micro laser patterning quality is not only influenced by the beam properties (beam profile, fluence) but also by pulse overlap, scan repetitions and many other factors such as substrate and coating material. This makes process parameter optimization a challengi…
Solvent-Directed Femtosecond Laser Ablation: Tuning Phase and Defect Engineering in Hybrid CdPS3/CdS Nanostructures
Moscow Center for Advanced Studies（莫斯科高级研究中心）；Frank Laboratory of Neutron Physics, Joint Institute for Nuclear Research（核物理弗兰克实验室，俄罗斯联合核研究所）；Emerging Technologies Research Center, XPANCEO（新兴技术中心，XPANCEO）；Department of General Physics, Perm National Research Polytechnic University（彼尔姆国立研究理工大学普通物理系）
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 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…
In this paper we analyze femtosecond laser processing of metals in liquids searching for optimal conditions for predictable ablation. Incident laser pulses are stretched or compressed, self-focused and scattered on bubbles and on surface waves in the liquid environment. Influence of these effects on the laser intensity distribution on the target surface is discussed and optimal processing parameters are suggested.
We present a new approach to femtosecond direct laser writing lithography to pattern nanocavities in ferromagnetic thin films. To demonstrate the concept we irradiated 300~nm thin nickel films by single intense femtosecond laser pulses through the glass substrate and created complex surface landscapes at the nickel-air interface. Using a fluence above the ablation threshold the process is destructive and irradiation leads to the formation of 200~nm thin flakes of nickel around the ablation crater as seen by electron microscopy. By progressively lowering the peak laser fluence, slightly below t…
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.
Powerful femtosecond laser pulses that propagate through narrow ablating capillaries cause modification of capillary walls, which is studied experimentally and theoretically. At low intensities, laser-induced periodic surface structures (LIPSS) and porous coating composed of sub-micron particles appear on the walls. At higher intensities, the surface is covered by deposited droplets of the size up to 10 $μ$m. In both cases, the ablated material forms a solid plug that completely blocks the capillary after several hundreds or thousands of pulses. The suggested theoretical model indicates that p…
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 …
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
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 provide measurements of ablation of four post-transition and transition metals (aluminum, copper, nickel and tungsten) irradiated by single 800 nm laser pulses, in ultrashort regime from 100 fs pulse duration down to 15 fs covering a temporal range little explored yet. For each metal and pulse duration tested, we measure its ablation characteristics (depth and diameter) as a function of incident energy allowing us to determine its laser-induced ablation threshold and ablation rate in single-shot regime. For all metals studied, we observe constant ablation threshold fluence as a function of …
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).
Dispersive wave emission (DWE) in gas-filled hollow-core dielectric waveguides is a promising source of tuneable coherent and broadband radiation, but so far the generation of few-femtosecond pulses using this technique has not been demonstrated. Using in-vacuum frequency-resolved optical gating, we directly characterise tuneable 3fs pulses in the deep ultraviolet generated via DWE. Through numerical simulations, we identify that the use of a pressure gradient in the waveguide is critical for the generation of short pulses.
Laser ablation in liquid (LAL) is important technique used for formation of nanoparticles (NP). The LAL processes cover logarithmically wide range of spatiotemporal scales and is not fully understood. The NP produced by LAL are rather expensive, thus optimization of involved processes is valuable. As the first step to such optimizations more deep understanding is necessary. We employ physical models and computer simulations by thermodynamic, hydrodynamic, and molecular dynamics codes in this direction. Absorbing light metal expanding into transparent solid or liquid dielectrics is considered. …
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 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 …
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…
