Ultrashort Laser Irradiation Research Articles

An advanced methodology for the development of highly accurate two temperature models (TTMs) to describe the material irradiation by an ultrashort laser

Ultrashort lasers are an evolving field in both the researching and industrial world, mainly due to their ability to give very small Heat Affected Zones (HAZ) during the irradiation of a material, making them efficient for micro- and nanostructuring. Two Temperature Models (TTMs) are widely used in literature to simulate the irradiation of a material by an ultrashort laser, however, still now, they have some significant limitations, such as boundary conditions and mesh size dependency and low accuracy in predicting ablation depth and crater diameter. The novelty of the current paper is that it proposes an advanced methodology for the development of heat transfer-only TTMs, with boundary conditions and mesh size independency, that are able to predict ablation depth and crater diameter with very high accuracy, as they take into consideration phenomena such as spallation, explosive boiling and Kerr effect. As an example, this methodology has been applied on the ultrashort laser irradiation of Au.

Study of the surface damage threshold and mechanism of KDP crystal under ultrashort laser irradiation

Here, we investigate the mechanism of surface damage threshold anisotropy induced by ultrashort laser in potassium dihydrogen phosphate (KDP) crystal. Carrier-lattice nonequilibrium interaction is simulated based on Brillouin light-scattering (BLS) spectroscopy and a complete self-consistent model to obtain the time evolution of carrier density and temperature as well as lattice temperature. The results indicate that the trend of the lattice temperature is consistent with the experimental phenomena. Meanwhile, the electron-phonon coupling effect, in addition to the electron density traditionally considered, is an important factor affecting damage and is a major contributor to the anisotropy of the damage threshold.

On the design and development of foamed GO-hydrogel nanocomposite surfaces by ultra-short laser processing

Graphene oxide (GO) and reduced graphene oxide have outstanding qualities that could be exploited as reinforcement and antibacterial agents in a plethora of biomedical applications. In this contribution, it is reported the deployment of a polyacrylamide GO-hydrogel composite (GO@pAAm) which was photo-converted and structured by ultra-short laser irradiation using a direct laser writing (DLW) approach. The materials were characterized by Fourier Transform Infrared spectroscopy, scanning electron microscopy and confocal microscopy. The laser structure generates a multi-photo-induced effect: surface foaming and patterning, microdomains with enhanced selective water-swelling and effective GO photo-reduction. A first laser scan seems likely to induce the photo-reduction of GO and subsequent laser pulses trigger the structure/foaming. The photo-reduction of GO is evidenced by Raman spectroscopy by the relatively changing intensities of the D to G signals. Macroscopically by an increase in conductivity (decrease in sheet resistance from R S-GO@pAAm = 304 ± 20 kΩ sq−1 to R S-rGO@pAAm-DLW = 27 ± 8 kΩ sq−1) suggesting a reduction of the material measured by 4-Point-Probe.

Creation of NV centers over a millimeter-sized region by intense single-shot ultrashort laser irradiation

Recently, ultrashort laser processing has attracted attention for creating nitrogen-vacancy (NV) centers because this method can create single NV centers in spatially-controlled positions, which is an advantage for quantum information devices. On the other hand, creating high-density NV centers in a wide region is also important for quantum sensing because the sensitivity is directly enhanced by increasing the number of NV centers. A recent study demonstrated the creation of high-density NV centers by irradiating femtosecond laser pulses, but the created region was limited to micrometer size, and this technique required many laser pulses to avoid graphitization of diamond. Here, we demonstrate the creation of NV centers in a wide region using only an intense single femtosecond laser pulse irradiation. We irradiated a diamond sample with a femtosecond laser with a focal spot size of 41 µm and a laser fluence of up to 54 J/cm2, which is much higher than the typical graphitization threshold in multi-pulse processing. We found that single-pulse irradiation created NV centers without post-annealing for a laser fluence higher than 1.8 J/cm2, and the region containing NV centers expanded with increasing laser fluence. The diameter of the area was larger than the focal spot size and reached over 100 µm at a fluence of 54 J/cm2. Furthermore, we demonstrated the NV centers’ creation in a millimeter-sized region by a single-shot defocused laser pulse over 1100 µm with a fluence of 33 J/cm2. The demonstrated technique will bring interest in the fundamentals and applications of fabricating ultrahigh-sensitivity quantum sensors.

Enhancement of ablation and ultrafast electron dynamics observation of nickel-based superalloy under double-pulse ultrashort laser irradiation

Temporally shaped femtosecond laser machining is a flexible and effective method to improve the efficiency and quality of cooling film holes. This study investigated the ablation of nickel-based superalloy by double-pulse femtosecond laser with different pulse-separations and fluences. Compared with single-pulse ablation, approximate 1.5 times enhancement of ablation area was obtained in double-pulse ablation with about 2 ps pulse-separation. By varying the pulse-separations, the ablation area can be tuned, and at the same time, the ablation depth can be kept for little fluctuation. An improved two-temperature model and time-resolved transient reflectivity technique were used for analyzing the ablation mechanisms. We found that more energy deposition can happen from electron system to lattice system for double-pulse ablation, which makes ablation area increase. However, mechanical relaxation started at around 2 ps, which could be suppressed by the pressure wave induced by the second sub-pulse, and finally achieved the maximum ablation area at about 2 ps pulse-separation. Besides, laser-induced subwavelength periodic surface structures were observed under irradiation of multiple pulses. The findings may aid in understanding the ablation mechanism between nickel-based superalloy and femtosecond laser, as well as in optimizing the processing of cooling film holes.

Investigating Potential Effects of Ultra-Short Laser-Textured Porous Poly-ε-Caprolactone Scaffolds on Bacterial Adhesion and Bone Cell Metabolism.

Developing antimicrobial surfaces that combat implant-associated infections while promoting host cell response is a key strategy for improving current therapies for orthopaedic injuries. In this paper, we present the application of ultra-short laser irradiation for patterning the surface of a 3D biodegradable synthetic polymer in order to affect the adhesion and proliferation of bone cells and reject bacterial cells. The surfaces of 3D-printed polycaprolactone (PCL) scaffolds were processed with a femtosecond laser (λ = 800 nm; τ = 130 fs) for the production of patterns resembling microchannels or microprotrusions. MG63 osteoblastic cells, as well as S. aureus and E. coli, were cultured on fs-laser-treated samples. Their attachment, proliferation, and metabolic activity were monitored via colorimetric assays and scanning electron microscopy. The microchannels improved the wettability, stimulating the attachment, spreading, and proliferation of osteoblastic cells. The same topography induced cell-pattern orientation and promoted the expression of alkaline phosphatase in cells growing in an osteogenic medium. The microchannels exerted an inhibitory effect on S. aureus as after 48 h cells appeared shrunk and disrupted. In comparison, E. coli formed an abundant biofilm over both the laser-treated and control samples; however, the film was dense and adhesive on the control PCL but unattached over the microchannels.

The role of fluence in determining the response of thin molybdenum films to ultrashort laser irradiation; from laser-induced crystallization to ablation via photomechanical ablation and nanostructure formation

The selective processing of Mo at low temperatures is challenging, especially in advanced manufacturing on flexible and heat-sensitive substrate due to its higher melting temperature. The key role of fluence in determining the response of thin Mo films to ultrashort laser irradiation is considered in this study. At low fluences, the electrical properties of Mo are enhanced by a localized laser-induced crystallization mechanism; the electrical mobility of Mo is increased and the contact resistance between Mo-Si interface is reduced. At higher fluences, selective patterning of Mo proceeds without impacting the Si layer and the threshold fluence for ablation increases with the film thickness of Mo. Two fluence dependent ablation mechanisms are observed depending on the Mo film thickness. For thin films of thicknesses 20 nm and 40 nm, selective ablation proceeds only by a photothermal interaction. For 60 nm and 80 nm thick films, selective ablation proceeds by both photomechanical and photothermal interactions at two-separate higher fluence regimes, respectively. Interestingly, between these two ablation regimes, a non-ablative nanostructuring regime occurs. The study provides a concise overview of the process window for implementing the laser-induced modifications to Mo layers with minimal impact to the substrate using single wavelength ultrashort pulse laser.

Ultrafast Laser Processing of Diamond Materials: A Review

Diamond laser engineering is of great importance for designing devices, which find applications in radiation sensing and quantum technologies. A review of the present state of the art of experimental and theoretical studies on ultrashort laser irradiation of diamond is presented. For a wide range of laser parameters, the optimization of laser-induced electronic, optical and structural modifications of diamond requires quantitative understanding of the microscopic processes underlying the high electronic excitation in the material.

Analysis of electromagnetic pulses generated from ultrashort laser irradiation of solid targets at CLAPA

Electromagnetic pulses (EMPs) produced by the interaction of a TW femtosecond laser with solid targets at the Compact Laser Plasma Accelerator (CLAPA) are measured and interpreted. The statistical results confirm that the intensities of the EMPs are closely related to both target material and thickness. The signal of the titanium target is more abundant than that of the copper target with the same thickness, and the intensity of EMP is positively correlated with the target thickness for aluminium foil. With the boosted EMP radiations, the energy of accelerated protons is also simultaneously enhanced. In addition, EMPs emitted from the front of the target exceed those from the rear, which are also pertinent to the specific target position. The resonant waveforms in the target chamber are analyzed using the fast Fourier transform, and the local resonance and the attenuation lead to changes of the frequency spectra of EMPs with variation of detecting positions, which is well supported by the modeling results. The findings are beneficial to gaining insight into the mechanism of EMP propagation in a typical target chamber and providing more information for EMP shielding design.

Electron Collision Rate in Ultrashort Laser – Metal Interaction Inferred from Reflectivity Measurements

We study optical laser coupling of four metals (aluminum, copper, nickel and tungsten) upon single ultrashort 30-fs laser irradiation. Using dedicated experimental methodology, we carefully monitor the evolution of the material reflectivity integrated over the femtosecond pulse duration. We further apply the Drude-Lorentz formalism to infer the evolution of the effective electron collision rate eff as a function of applied fluence. The knowledge of this parameter is of paramount importance in any lasermatter interaction situation because of its immediate impact on laser energy coupling in material and on its subsequent macroscopic transformation.

Transient optics of gold during laser irradiation: From first principles to experiment

The reflectivity of noble metals can dramatically change upon ultrashort laser irradiation due to the heating of $d$ electrons to high temperatures. Knowledge of the resulting transient optics is fundamental for determining and controlling the absorbed energy. In this work, high-accuracy self-reflectivity measurements are performed and interpreted using a theory for the space-resolved and time-resolved energy absorption and dissipation. The combined approach yields the reflectivity of gold in dependence on the incident laser fluence for a wide spectral range.

Ultra-short laser-induced high aspect ratio densification in porous glass

Multiple ultra-short laser irradiation enabling direct writing of high aspect ratio barriers is used for structuring of nanoporous glass. Shape and morphology of laser-modified regions are examined, and high aspect ratio laser-induced material densification is founded. Experimental results are analyzed by modeling describing laser propagation, non-linear ionization and thermal effects. The role of laser focusing, laser energy and pulse number are examined. Several regimes are distinguished. Particularly, high-aspect ratio densified zones are obtained for the numerical aperture of 0.25, whereas either more symmetric densified regions or spherical cavities are shown to be formed for numerical aperture of 0.4. The resulting laser irradiation conditions required for deep and prolonged densification are explained by a lower ionization rate, leading to the under-critical free electron plasma density, longer filamentation and pulse-to-pulse elongation effects. Furthermore, filling of the porous glass with water is demonstrated to particularly extend the length of the densified region in depth. The presented study provides insights facilitating laser-based fabrication of barriers, membrane and patterns suitable for the environmental gas-phase analysis.

Material evaporation with ultrashort laser exposure

The task is to analyse the temperature distribution in the material under ultrashort laser irradiation. The mathematical model is built on the basis of a two-temperature model describing transition phenomena in a nonequilibrium electron gas and lattice with an ultrashort laser effect on the material. The vaporized body is considered as a thin plate and the problem is formulated as a system of one-dimensional boundary-value problems of the heat equation written for the electron and lattice components. The initial problem is reduced to solving a system of singularly perturbed boundary problems of the heat equation with nonlinear boundary conditions on moving boundaries, an approximate solution of which is obtained in the form of an asymptotic expansion of the solution in the Poincaré sense in powers of small parameters.

Ablation enhancement of metal in ultrashort double-pulse experiments

We report an ablation enhancement (both deepening and widening in ablation profiles) on nickel by ultrashort double-pulse laser irradiation, an exception of the typical reduction trend observed in ablation rates for metals irradiated with double-pulse excitations. Maximized at a pulse-separation (τs) of approximately 4 ps, the enhancement was observed before τs was increased to approximately the electron-lattice energy relaxation time. An achievement of ablation, by temporal shaping a weak pulse with energy well below the single-pulse ablation threshold into two considerably weaker pulses, was demonstrated. It is proposed that the enhanced electron-phonon coupling and drop of electronic heat conductivity, both of which result from the reductions in electron temperature (by pulse shaping), co-contribute to the widening in ablation profiles, while the former one is responsible for the deepening. This letter proposed an ablation enhancement approach to ultrashort laser processing of nickel.

Femtosecond laser irradiation of olivine single crystals: Experimental simulation of space weathering

Space weathering is one of the most common surface process occurring on atmosphere-free bodies such as asteroids and the Moon. It is caused mainly by solar wind irradiation and the impact of micrometeoroids. In order to simulate space weathering effects, in particular those produced by hypervelocity impacts, we produced microcraters via ultra-short (∼100 fs) laser irradiation of crystallographically oriented slices of forsterite-rich (Fo94.7) olivine. The main advantages of the application of a femtosecond laser radiation to reproduce the space weathering effects are (1) the high peak irradiance (1015 W cm−2), which generates the propagation of the shock wave at the nanosecond timescale (i.e., timescale of the micrometeoroid impacts); (2) the rapid transfer of energy to the target material, which avoids the interaction of laser light with the developing vapor plume; (3) a small laser beam, which allows the effects of a single impact to be simulated. The results of our spectroscopic and electron microscopic investigation validate this approach: the samples show strong darkening and reddening of the reflectance spectra and structural damages similar to the natural microcraters found on regolith grains of the Moon and asteroid 25143 Itokawa. Detailed investigations of several microcrater cross-sections by transmission electron microscopy allowed the detection of shock-induced defect microstructures. From the top to the bottom of the grain, the shock wave causes evaporation, melting, solid-state recrystallization, misorientation, fracturing, and the propagation of dislocations with Burgers vectors parallel to [001]. The formation of a short-lived vapor plume causes the kinetic fractionation of the gas and the preferential loss of lighter elements, mostly magnesium and oxygen. The high temperatures within the melt layer and the kinetic loss of oxygen promote the thermal reduction of iron and nickel, which leads to the formation of metallic nanoparticles (npFe0). The final stage of the microcrater formation is the cooling of the melt layer that results in its partial crystallization and the formation of olivine crystals with a palisade-like texture.

Silica Xerogel Obtained by Ultrashort Laser Irradiation of Tetraethyl Orthosilicate.

The formation of an opaque solid foam was induced by the direct interaction between tetraethyl orthosilicate (TEOS) and an ultrashort femtosecond laser source(Nd:glass, 527 nm, 10 Hz, 250 fs). The product, which resulted to be a silica xerogel, was characterized by different techniques. In particular, information about the morphology was obtained by scanning and transmission electron microscopy (SEM and TEM), while the presence of different functional groups was studied through IR measurements. Since the properties of this kind of material can be improved by functionalizing it with metal nanoparticles, a palladium metal target was ablated in liquid TEOS. TEM images show that palladium was present in the form of nanoparticles and EDX measurements confirm the presence of the metal inside the silica network.

Simulation of ablation and plume dynamics under femtosecond double-pulse laser irradiation of aluminum: Comparison of atomistic and continual approaches

We elaborated two numerical methods, two-temperature hydrodynamics and hybrid two-temperature molecular dynamics, which take into account basic mechanisms of a metal target response to ultrashort laser irradiation. The model used for the description of the electronic subsystem is identical for both approaches, while the ionic part is defined by an equation of state in hydrodynamics and by an interatomic potential in molecular dynamics. Since the phase diagram of the equation of state and corresponding potential match reasonably well, the dynamics of laser ablation obtained by both methods is quite similar. This correspondence can be considered as a first step towards the development of a self-consistent combined model. Two important processes are highlighted in simulations of double-pulse ablation: (1) the crater depth decrease as a result of recoil flux formation in the nascent plume when the delay between the pulses increases; (2) the plume reheating by the second pulse that gives rise to two- three-fold growth of the electron temperature with the delay varying from 0 to 200ps.

Preliminary study of surface modification of 3D Poly (ɛ - caprolactone) scaffolds by ultrashort laser irradiation

Three - dimensional poly (e- caprolactone) (PCL) scaffolds as suitable biocompatible material for manufacturing tissue replacements are utilized for tissue engineering purposes. The porous structures are fabricated by rapid prototyping method (Bioscaffolder) based on hypodermic dispensing process. The consecution of experiments demonstrated the possibility on creation of surface micro formations, applying different laser fluences, at 1 kHz repetition rate for fixed time of exposure 1 sec at 800 nm central wavelength. The combination of both methods offers possibilities for successful production of 3D matrices with modified surfaces. The obtained results of laser - induced surface modifications of PCL demonstrate the potential of the method to microprocess this kind of material for possible applications in regenerative medicine.

Nonlocal two-temperature model: Application to heat transport in metals irradiated by ultrashort laser pulses

Extended two-temperature models with allowance for time (relaxation) and space nonlocal effects have been developed to describe, in particular, heat conduction in metals under ultrashort laser irradiation, which overheats the electron gas in comparison with the lattice leading to energy exchange between them. The time nonlocal effects arise when the electron gas is driven out of local (thermal) equilibrium, whereas the space nonlocal effects begin to be significant when the spatial extent of the temperature gradient is comparable with the mean-free path of the heat carrier. The electron-lattice energy exchange as well as the space–time nonlocal effects in the electron gas leads to a hierarchy of space–time nonlocal heat conduction equations for the electron and lattice temperatures, which are partial differential equation of higher order in comparison with the classical heat conduction equation. The models presented here may be used in combination with molecular dynamic and phase-field approaches.

Laser-Induced Plasma Micromachining Process: Principles and Performance

Laser-induced plasma micromachining (LIP-MM) is a novel multimaterial and tool-less micromachining process. It utilizes tightly focused ultrashort laser irradiation to generate plasma through laser-induced dielectric breakdown in a dielectric material. The plasma facilitates material removal through plasma–matter interaction spot through vaporization and ablation. The paper introduces the LIP-MM process, discusses the underlying principles behind plasma generation and machining, and proves its feasibility by describing the experimental conditions under which plasma generation and machining occur. Upon successful commercial realization of this novel process, the key benefits envisaged are micromachining with better accuracy and better surface integrity, minimal subsurface damage, relatively smaller heat-affected zone (HAZ) and low roughness in a wide range of materials including those that are difficult to machine by some of the most successful micromachining processes such as micro-electrodischarge machining (EDM) and laser ablation.