Thermal melting and ablation dynamics on a femtosecond laser-heated highly-oriented pyrolytic graphite surface

Time-resolved optical reflection microscopy studies demonstrate spatiotemporal dynamics of melting and ablation of graphite surface molten by single IR femtosecond laser pulses, which are revealed by monitoring picosecond oscillations of the probe reflectivity modulated by transient acoustic reverberations in the surface melt. Temporal periods and amplitudes of the reverberations are affected through transient variations of melt thickness and acoustic impedance by melting, thermal expansion, spallation and fragmentation processes, thus enabling quantitative evaluation of their contributions and basic parameters.     

Thermal melting and ablation of silicon by femtosecond laser radiation

The space-time dynamics of thermal melting, subsurface cavitation, spallative ablation, and fragmentation ablation of the silicon surface excited by single IR femtosecond laser pulses is studied by timeresolved optical reflection microscopy. This dynamics is revealed by monitoring picosecond and (sub)nanosecond oscillations of probe pulse reflection, which is modulated by picosecond acoustic reverberations in the dynamically growing surface melt subjected to ablation and having another acoustic impedance, and by optical interference between the probe pulse replicas reflected by the spalled layer surface and the layer retained on the target surface. The acoustic reverberation periods change during the growth and ablation of the surface melt film, which makes it possible to quantitatively estimate the contributions of these processes to the thermal dynamics of the material surface. The results on the thermal dynamics of laser excitation are supported by dynamic measurements of the ablation parameters using noncontact ultrasonic diagnostics, scanning electron microscopy, atomic force microscopy, and optical interference microscopy of the modified regions appearing on the silicon surface after ablation.     

Nanoscale cavitation instability of the surface melt along the grooves of one-dimensional nanorelief gratings on an aluminum surface

Femtosecond laser nanostructuring at low fluences produces a one-dimensional quasiperiodic grating of grooves on an aluminum surface with a period (≈0.5 μm) that is determined by the length of a surface electromagnetic wave. The structure of the grooves of the surface nanograting is formed by regular nanopeaks following with a period of about 200 nm. Some nanopeaks manifest craters at their tops. It is suggested that nanopeaks are formed due to the frozen nanoscale spallative ablation of a nanolayer of an aluminum melt in quasiperiodic regions corresponding to interference maxima of the laser radiation with the surface electromagnetic wave. The periodicity of the appearance of nanopeaks along grooves is due to the previously predicted mechanism of cavitation deformation of the melt surface in the process of macroscopic spallation ablation. However, in this case, cavitation is coherent (similar to a near-critical spinodal decay) rather than spontaneous.     

Modeling the dynamics of one laser pulse surface nanofoaming of biopolymers

Self standing films of biopolymers like gelatine, collagen, and chitosan irradiated with single nanosecond or femtosecond laser pulse easily yield on their surface, a nanofoam layer, formed by a cavitation and bubble growth mechanism. The laser foams have interesting properties that challenge the molecular features of the natural extracellular matrix and which make them good candidates for fabrication of artificial matrix (having nanoscopic fibers, large availability of cell adhesion sites, permeability to fluids due to the open cell structure). As part of the mechanistic study, the dynamics of the process has been measured in the nanosecond timescale by recording the optical transmission of the films at 632.8 nm during and after the foaming laser pulse. A rapid drop 100→0% taking place within the first 100 ns supports the cavitation mechanism as described by the previous negative pressure wave model. As modeled a strong pressure rise (∼several thousands of bar) first takes place in the absorption volume due to pressure confinement and finite sound velocity, and then upon relaxation after some delay equal to the pressure transit time gives rise to a rarefaction wave (negative pressure) in which nucleation and bubble growth are very fast.     

New mechanism of the formation of the nanorelief on a surface irradiated by a femtosecond laser pulse

The kinetics of fast processes induced by an ultrashort laser pulse is considered. The reliefs remaining after the action of a series of ultrashort laser pulses {S. A. Akhmanov, V. I. Emelyanov, N. I. Koroteev, et al., Usp. Fiz. Nauk 147, 675 (1985) [Sov. Phys. Usp. 28, 1084 (1985)]; F. Costache, S. Kouteva-Arguirova, and J. Reif, Appl. Phys. A 79, 1429 (2004)} have been studied. A new mechanism of perturbing the surface of the initially ideal crystal face is described. First, the formation of a relief is induced by a single pulse. Second, the relief scale along the target surface is about the heating depth d _T ～ 10–100 nm rather than the pump-pulse wavelength λ_pump ～ 1 μm. Third, the formation of the relief is not attributed to the modulation of the electromagnetic field near the surface due to the interference of the incident light wave with the electromagnetic surface waves on the initial perturbations of the boundary. These three conditions are satisfied for a known instability induced by the interference of the incident and surface waves (see the works cited above [1]). In our case, the nanorelief is formed due to the deformation of the spalled layer by cavitation bubbles owing to the inhomogeneity of the drag force in the target plane. Cavitation is caused by the tension of the substance in the process of the expansion of a heated target. It is similar to the known phenomenon of the cavitation “spallation” in a liquid despite the large difference between the space-time scales of the usual spallation facility and the femtosecond heating. Owing to this difference, usual cavitation does not leave any morphological trace on the outer free surface of the spalled layer.     

Acoustic substrate expansion in modelling dry laser cleaning of low absorbing substrates

Acoustic expressions have been derived for the thermal expansion of substrate surfaces due to irradiation by an exponential laser pulse. The result of acoustic effects on three substrates (silicon, glass and silica) with different absorptions has been calculated.It has been shown that for substrates having relatively low absorptions, like silica and glass, acoustic considerations substantially reduce thermal expansion of the substrate caused by irradiation by nanosecond laser pulses relative to a quasi-static expansion model. In particular, the expansion of the substrate occurs over a much longer time frame than when the quasi-static approximation holds. Consequently, acceleration of the substrate surface is greatly reduced and laser cleaning threshold fluences for particle removal are increased.The predictions of the model of Arnold et al. when developed for acoustic considerations give reasonable agreement with experimentally found threshold fluences for alumina particles on silica and glass substrates although it underestimates the ratio of the threshold cleaning fluences of silica and glass. This could be due to the model underestimating the contribution of surface expansion to the laser cleaning process. The influence of multiple reflections in the substrate and departure from one dimensionality in the heat conduction on the threshold fluence was found to be insignificant. Thermal contact between the particle and the substrate was also found to have little effect on laser cleaning threshold fluences. Another mechanism that may enhance surface expansion is the 3D focussing of radiation by the particles. PACS 42.62.Cf; 81.65.Cf; 42.55.Lt     

Short-laser-pulse-driven emission of energetic ions into a solid target from a surface layer spalled by a laser prepulse

An efficient emission of picosecond bunches of energetic protons and carbon ions from a thin layer spalled from a organic solid by a laser prepulse is demonstrated numerically. We combine the molecular dynamics technique and multi-component collisional particle-in-cell method with plasma ionization to simulate the laser spallation and ejection of a thin (∼20–30 nm) solid layer from an organic target and its further interaction with an intense femtosecond laser pulse. In spite of its small thickness, a layer produced by laser spallation efficiently absorbs ultrashort laser pulses with the generation of hot electrons that convert their energy to ion energy. The efficiency of the conversion of the laser energy to ions can be as high as 20%, and 10% to MeV ions. A transient electrostatic field created between the layer and surface of the target is up to 10 GV/cm. Received: 13 March 2001 / Accepted: 20 March 2001 / Published online: 20 June 2001     

Spallative ablation of dielectrics by X-ray laser

A short laser pulse in wide range of wavelengths, from infrared to X-ray, disturbs electron–ion equilibrium and increases pressure in a heated layer. The case where the 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 of wavelength. While the physics of electron–ion relaxation strongly depends 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 metals. The paper describes entire sequence of thermomechanical processes from expansion, nucleation, foaming, and nanostructuring to spallation with particular attention to spallation by X-ray pulse.     

Characterization of acoustic streaming in water and aluminum melt during ultrasonic irradiation

It is well known that ultrasonic cavitation causes a steady flow termed acoustic streaming. In the present study, the velocity of acoustic streaming in water and molten aluminum is measured. The method is based on the measurement of oscillation frequency of Karman vortices around a cylinder immersed into liquid. For the case of acoustic streaming in molten metal, such measurements were performed for the first time. Four types of experiments were conducted in the present study: (1) Particle Image Velocimetry (PIV) measurement in a water bath to measure the acoustic streaming velocity visually, (2) frequency measurement of Karman vortices generated around a cylinder in water, and (3) in aluminum melt, and (4) cavitation intensity measurements in molten aluminum. Based on the measurement results (1) and (2), the Strouhal number for acoustic streaming was determined. Then, using the same Strouhal number and measuring oscillation frequency of Karman vortices in aluminum melt, the acoustic streaming velocity was measured. The velocity of acoustic streaming was found to be independent of amplitude of sonotrode tip oscillation both in water and aluminum melt. This can be explained by the effect of acoustic shielding and liquid density.     

Laser-induced cavitation bubbles and shock waves in water near a concave surface

The interplay among the cavitation structures and the shock waves following a nanosecond laser breakdown in water in the vicinity of a concave surface was visualized with high-speed shadowgraphy and schlieren cinematography. Unlike the generation of the main cavitation bubble near a flat or a convex surface, the concave surface refocuses the emitted shock waves and causes secondary cavitation near the acoustic focus which is most pronounced when triggered by the shock wave released during the first main bubble collapse. The shock wave propagation, reflection from the concave surface and its scattering on the dominant cavity is clearly resolvable on the shadowgraphs. The schlieren approach revealed the pressure build up in the last stage of the collapse and the first stage of the rebound. A persistent low-density watermark is left behind the first collapse. The observed effects are important wherever cavities collapse near indented surfaces, such as in cavitation peening, cavitation erosion and ophthalmology.     

Identification approach of acoustic cavitation via frequency spectrum of sound pressure wave signals in numerical simulation

In a sono-reactor, complex ultrasound pressure wave signal can be detected, containing multiple information related to acoustic cavitation. In this present study, acoustic cavitation in a cylinder is investigated numerically. Via Fast Fourier Transfer (FFT), the sound pressure signals from sonotrode emitting surface are separated into harmonics, sub/ultra-harmonics and cavitation white noise: (1) the appearance of harmonics proved the non-linear propagation of ultrasound, (2) at the vibratory amplitude from 5∼20μm, only harmonics exists in the frequency spectra, corresponding to expansion and compression of non-condensable gas (NCG), (3) at the vibratory amplitude range of 30∼50μm, the occurrence of sub/ultra-harmonics demonstrated gaseous cavitation occurred, and (4) at the vibratory amplitude higher than 55μm, cavitation white noise arose, pointing out the initiation of vaporous cavitation. Based on the combination of frequency spectra and cavitation zones distribution, the acoustic cavitation state in water liquid is determined.     

Efficient and controllable thermal ablation induced by short-pulsed HIFU sequence assisted with perfluorohexane nanodroplets

A HIFU sequence with extremely short pulse duration and high pulse repetition frequency can achieve thermal ablation at a low acoustic power using inertial cavitation. Because of its cavitation-dependent property, the therapeutic outcome is unreliable when the treatment zone lacks cavitation nuclei. To overcome this intrinsic limitation, we introduced perfluorocarbon nanodroplets as extra cavitation nuclei into short-pulsed HIFU-mediated thermal ablation. Two types of nanodroplets were used with perfluorohexane (PFH) as the core material coated with bovine serum albumin (BSA) or an anionic fluorosurfactant (FS) to demonstrate the feasibility of this study. The thermal ablation process was recorded by high-speed photography. The inertial cavitation activity during the ablation was revealed by sonoluminescence (SL). The high-speed photography results show that the thermal ablation volume increased by ∼643% and 596% with BSA-PFH and FS-PFH, respectively, than the short-pulsed HIFU alone at an acoustic power of 19.5 W. Using nanodroplets, much larger ablation volumes were created even at a much lower acoustic power. Meanwhile, the treatment time for ablating a desired volume significantly reduced in the presence of nanodroplets. Moreover, by adjusting the treatment time, lesion migration towards the HIFU transducer could also be avoided. The SL results show that the thermal lesion shape was significantly dependent on the inertial cavitation in this short-pulsed HIFU-mediated thermal ablation. The inertial cavitation activity became more predictable by using nanodroplets. Therefore, the introduction of PFH nanodroplets as extra cavitation nuclei made the short-pulsed HIFU thermal ablation more efficient by increasing the ablation volume and speed, and more controllable by reducing the acoustic power and preventing lesion migration.     

Molecular dynamics simulation of femtosecond ablation and spallation with different interatomic potentials

Fast heating of target material by femtosecond laser pulse (fsLP) with duration τ_L∼40-100 fs results in the formation of thermomechanically stressed state. Its unloading may cause frontal cavitation of subsurface layer at a depth of 50 nm for Al and 100 nm for Au. The compression wave propagating deep into material hits the rear-side of the target with the formation of rarefaction wave. The last may produce cracks and rear-side spallation. Results of MD simulations of ablation and spallation of Al and Au metals under action fsLP are presented. It is shown that the used EAM potentials (Mishin et al. and our new one) predict the different ablation and spallation thresholds on absorbed fluence in Al: ablation F_a=60{65} mJ/cm²and spallation F_s=120{190} mJ/cm², where numbers in brackets { } show the corresponding values for Mishin potential. The strain rate in spallation zone was 4.3×10⁹ 1/s at spallation threshold. Simulated spall strength of Al is 7.4{8.7} GPa, that is noticeably less than 10.3{14} GPa obtained from acoustic approximation with the use of velocity pullback on velocity profile of free rear surface. The ablation threshold F_a≈120 mJ/cm² and crater depth of 110 nm are obtained in MD simulations of gold with the new EAM potential. They agree well with experiment.     

Ultrasonic cavitation at liquid/solid interface in a thin Ga–In liquid layer with free surface

Cavitation in thin layer of liquid metal has potential applications in chemical reaction, soldering, extraction, and therapeutic equipment. In this work, the cavitation characteristics and acoustic pressure of a thin liquid Ga–In alloy were studied by high speed photography, numerical simulation, and bubble dynamics calculation. A self-made ultrasonic system with a TC4 sonotrode, was operated at a frequency of 20 kHz and a max output power of 1000 W during the cavitation recording experiment. The pressure field characteristic inside the thin liquid layer and its influence on the intensity, types, dimensions, and life cycles of cavitation bubbles and on the cavitation evolution process against experimental parameters were systematically studied. The results showed that acoustic pressure inside the thin liquid layer presented alternating positive and negative characteristics within 1 acoustic period (T). Cavitation bubbles nucleated and grew during the negative-pressure stage and shrank and collapsed during the positive-pressure stage. A high bubble growth speed of 16.8 m/s was obtained and evidenced by bubble dynamics calculation. The maximum absolute pressure was obtained at the bottom of the thin liquid layer and resulted in the strongest cavitation. Cavitation was divided into violent and weak stages. The violent cavitation stage lasted several hundreds of acoustic periods and had higher bubble intensity than the weak cavitation stage. Cavitation cloud preferentially appeared during the violent cavitation stage and had a life of several acoustic periods. Tiny cavitation bubbles with life cycles shorter than 1 T dominated the cavitation field. High cavitation intensities were observed at high ultrasonication power and when Q235B alloy was used because such conditions lead to high amplitudes on the substrate and further high acoustic pressure inside the liquid.     

Thermocavitation melt instability and micro-crown formation near the threshold for femtosecond laser spallation of a silicon surface

Thermocavitation instability of a molten layer on a silicon surface was experimentally revealed in the form of a microscale surface crown-like feature produced by multiple infrared or visible femtosecond laser pulses near the spallation threshold fluence. The number of crown spikes varied versus the crown perimeter, monotonically increasing with increasing laser shot number. The instability dynamics was described in terms of the intermediate crown structures (the spike number) using the proposed thermocavitation model based on the Kuramoto-Sivashinsky hydrodynamic equation.     

Characterisation of the acoustic cavitation cloud by two laser techniques

An experimental investigation of the size and volumetric concentration of acoustic cavitation bubbles is presented. The cavitation bubble cloud is generated at 20 kHz by an immersed horn in a rectangular glass vessel containing bi-distilled water. Two laser techniques, laser diffraction and phase Doppler interferometry, are implemented and compared. These two techniques are based on different measuring principles. The laser diffraction technique analyses the light pattern scattered by the bubbles along a line-of-sight of the experimental vessel (spatial average). The phase Doppler technique is based on the analysis of the light scattered from single bubbles passing through a set of interference fringes formed by the intersection of two laser beams: bubble size and velocity distributions are extracted from a great number of single-bubble events (local and temporal average) but only size distributions are discussed here. Difficulties arising in the application of the laser diffraction technique are discussed: in particular, the fact that the acoustic wave disturbs the light scattering patterns even when there are no cavitation bubbles along the measurement volume. As a consequence, a procedure has been developed to correct the raw data in order to get a significant bubble size distribution. After this data treatment has been applied the results from the two measurement techniques show good agreement. Under the emitter surface, the Sauter mean diameter D(3, 2) is approximately 10 microm by phase Doppler measurement and 7.5 microm by laser diffraction measurement at 179 W. Note that the mean measured diameter is much smaller than the resonance diameter predicted by the linear theory (about 280 microm). The influence of the acoustic power is investigated. Axial and radial profiles of mean bubble diameters and void fraction are also presented.     

Microscopic mechanisms of short pulse laser spallation of molecular solids

The mechanisms of photomechanical spallation are investigated in a large-scale MD simulation of laser interaction with a molecular target performed in an irradiation regime of inertial stress confinement. The relaxation of laser-induced thermoelastic stresses is found to be responsible for the nucleation, growth, and coalescence of voids in a broad sub-surface region of the irradiated target. The depth of the region subjected to void evolution is defined by the competition between the evolving tensile stresses and thermal softening of the material due to the laser heating. The initial void volume distribution obtained in the simulation of laser spallation can be well described by a power law. A similar volume distribution is obtained in a series of simulations of uniaxial expansion of the same molecular system performed at a strain rate and temperature realized in the irradiated target. Spatial and time evolution of the laser-induced pressure predicted in the MD simulation of laser spallation is related to the results of an integration of a thermoelastic wave equation. The scope of applicability of the continuum calculations is discussed. PACS 79.20.Ds; 61.80.Az; 02.70.Ns; 83.60.Uv     

液体薄层中的超声空化*

液体薄层中的超声空化,因其边界及所处空间的特殊性,而呈现出非常独特的空化结构和演化行为,在超声清洗、超声钎焊、表面处理、近场声悬浮、超声化学等领域都有所应用。该文梳理了近几年该课题组在液体薄层中的超声空化研究中的一些成果,力图揭示液体薄层内空泡、空化云、空化场的运动和分布规律,及其产生、发展和演化过程,以期对液体薄层中的超声空化行为有一个相对清晰和完整的认识。     

3-D finite element modeling of laser cladding by powder injection: effects of laser pulse shaping on the process

This paper introduces a 3-D transient finite element model of laser cladding by powder injection to investigate the effects of laser pulse shaping on the process. The proposed model can predict the clad geometry as a function of time and process parameters including laser pulse shaping, travel velocity, laser pulse energy, powder jet geometry, and material properties. In the proposed strategy, the interaction between powder and melt pool is assumed to be decoupled and as a result, the melt pool boundary is first obtained in the absence of powder spray. Once the melt pool boundary is obtained, it is assumed that a layer of coating material is deposited on the intersection of the melt pool and powder stream in the absence of the laser beam in which its thickness is calculated based on the powder feedrate and elapsed time. The new melt pool boundary is then calculated by thermal analysis of the deposited powder layer, substrate and laser heat flux. The process is simulated for different laser pulse frequencies and energies. The results are presented and compared with experimental data. The quality of clad bead for different parameter sets is experimentally evaluated and shown as a function of effective powder deposition density and effective energy density. The comparisons show excellent agreement between the modeling and experimental results for cases in which a high quality clad bead is expected.     

Characterization of cavitation under ultrasonic horn tip – Proposition of an acoustic cavitation parameter

Acoustic cavitation, generated by a piezo-driven transducer, is a commonly used technique in a variety of processes, from homogenization, emulsification, and intensification of chemical reactions to surface cleaning and wastewater treatment. An ultrasonic horn, the most commonly used acoustic cavitation device, creates unique cavitation conditions under the horn tip that depend on various parameters such as the tip diameter, the driving frequency of the horn, its amplitude, and fluid properties. Unlike for hydrodynamic cavitation, the scaling laws for acoustic cavitation are poorly understood. Empirical relationships between cavitation dynamics, ultrasonic horn operating conditions, and fluid properties were found through systematic characterization of cavitation under the tip. Experiments were conducted in distilled water with various sodium chloride salt concentrations under different horn amplitudes, tip geometries, and ambient pressures. Cavitation characteristics were monitored by high-speed (200,000 fps) imaging, and numerous relations were found between operating conditions and cavitation dynamics. The compared results are discussed along with a proposal of a novel acoustic cavitation parameter and its relationship to the size of the cavitation cloud under the horn tip. Similar to the classical hydrodynamic cavitation number, the authors propose for the first time an acoustic cavitation parameter based on experimental results.