Angular distributions of plume components in ultrafast laser ablation of metal targets

In view of its fundamental interest and relevance to nanoparticle film production, we have characterised the nanoparticle component of the ablation plume generated in femtosecond laser irradiation of metals. The results are compared to those of the ion plume, which is considered as representative of the atomic component. At moderate laser fluences, the angular distributions of both nanoparticle and ionic components were studied by measuring the spatial distribution of deposition on a transparent substrate and with a planar Langmuir probe, respectively. Our results show that both angular profiles of the plume components can be described by Anisimov model of isentropic expansion. As the laser fluence is increased above a value of several times the ablation threshold, the shape of the nanoparticle angular distribution progressively differs from the Anisimov prediction, contrary to what is observed for the ion component. This effect is interpreted in terms of the influence of the pressure exerted by the nascent atomic plasma plume on the initial hydrodynamic evolution of nanoparticle material.     

Absolute phase effect in ultrafast optical responses of metal nanostructures

We predict that nonlinear ultrafast electron photoemission by strong optical fields and, potentially, other nonlinear optical responses of metal nanostructures significantly depend on the absolute (carrier–envelope) phase of excitation pulses. Strong enhancement of the local optical fields produces these responses at excitation intensities lower by order(s) of magnitude than for known systems. Prospective applications include control of ultrafast electron emission and electron injection into nanosystems. A wider class of prospective applications is the determination of the absolute phase of pulses emitted by lasers and atoms, molecules, and condensed matter at relatively low intensities. PACS  78.67.-n; 78.47.+p; 79.60.Jv; 73.20.Mf     

Laser backwriting process on glass via ablation of metal targets

Ablation of metal targets onto pyrex glass substrates, using a Q-switched Nd:YAG laser working at 355 nm, was used to study the potential of a laser backwriting process for the fabrication of optical waveguides via an index of refraction change. Metal foils of stainless steel, aluminum, copper, brass and gold have been used as blanks and irradiated by focusing the laser beam through a cylindrical lens under continuous movement in a direction perpendicular to the irradiation. An horizontal setup was found suitable to improve the effect of the plume in the sample. Results were obtained for two different configurations. Transversal profiles were analysed using a contact profilometer, comparing results obtained for the different configurations, traverse speeds and metal targets used. Two ablation regimes were identified, which are related to a critical laser fluence value of 2.7 J/cm². Surface micrographs obtained by scanning electron microscopy are discussed, together with the characteristics of the structures attained, taking into account the optical and thermal properties of the ablated metal blanks.     

Short-pulse laser ablation of solids: from phase explosion to fragmentation

The mechanisms of laser ablation in silicon are investigated close to the threshold energy for pulse durations of 500 fs and 50 ps. This is achieved using a unique model coupling carrier and atom dynamics within a unified Monte Carlo and molecular-dynamics scheme. Under femtosecond laser irradiation, isochoric heating and rapid adiabatic expansion of the material provide a natural pathway to phase explosion. This is not observed under slower, nonadiabatic cooling with picosecond pulses where fragmentation of the hot metallic fluid is the only relevant ablation mechanism.     

Nonlinearity and time-resolved studies of ion emission in ultrafast laser ablation of graphite

We have investigated the laser fluence dependence of the ion emission process in ultrafast laser ablation of graphite using a time-of-flight technique. Two regimes of ion emission have been identified: (1) a highly nonlinear laser absorption process accompanied by generation of a transient electrical field on the surface and collisionless emission of ions due to electrostatic repulsion; (2) a saturation regime for laser power absorption characterised by nearly equal kinetic energy of ejected carbon clusters. We also show the effect of the surface temperature on the emitted clusters’ stability and the influence of nonlinearity on the intensity autocorrelation traces.     

Pulsed laser ablation of solids: transition from normal vaporization to phase explosion

We present experimental data on mass removal during 1064-nm pulsed laser ablation of graphite, niobium and YBa₂Cu₃O_7-δ superconductor. Evidence for the transition from normal vaporization to phase explosion has been obtained for these materials, showing a dramatic increase in the ablation rate at the threshold fluences of 22, 15 and 17.5 J/cm², respectively. A numerical model is used to evaluate the ablation rate and temperature distribution within the targets under near-threshold ablation conditions. The results are analyzed from the viewpoint of the vaporized matter approaching the critical point with increasing laser fluence. A possible means of the estimating the thermodynamic critical temperature from the data for nanosecond laser ablation is discussed. It is suggested that the critical temperature of refractory metals is higher than that estimated with the traditional methods due to plasma effects. An analogy with the boiling crisis (the transition from nucleate to film boiling) is drawn to explain the formation of ablation craters with spallated edges. Received: 18 May 2000 / Accepted: 14 July 2000 / Published online: 22 November 2000     

Theoretical studies of adatom diffusion on metal surfaces

We propose in this paper a theoretical model to investigate surface self-diffusion of single adatoms on two different low-index planes, closely packed (001) and densely packed (111), of face-centered-cubic rhodium, nickel and copper metal crystals. Two realistic model potentials are applied to describe the interatomic interaction of the adatom-substrate systems. The first model is a Morse-type potential, which involves several empirical fittings of bulk of solid. The second, newly popular, potential was introduced by Sutton and Che, which incorporates many-body effects. With these potentials, conventional molecular dynamics (MD) is employed to obtain trajectories of the atoms. The average squared didplacements are computed for a range of initial kinetic energies, and the surface diffusion constants can be obtained by means of the Einstein relation. The estimated random walk exponential prefactors and activation energies exhibit an Arrhenius behavior, and are compared with previous results.     

Theoretical description of ultrafast phenomena in clusters

A theoretical study of different ultrafast nonequilibrium processes taking place during and after ultrashort excitation of clusters is presented. We discuss similarities and differences for several processes involving nonequilibrium ultrafast motion of atoms and electrons. We study ultrashort relaxation of clusters in response to excitations produced by femtosecond laser pulses of different intensities. We show how different relaxation processes, such as bond breaking, melting, fragmentation, emission of atoms, or Coulomb explosion, can be induced, depending on the laser intensity and laser pulse duration. We also discuss processes involving nonequilibrium electron dynamics, such as intraband Auger decay in clusters and ultrafast electronic motion during collisions between clusters and surfaces. We show that this electron dynamics leads to Stückelberg-like oscillations of measurable quantities, such as the electron emission yield. Received: 4 April 2000 / Accepted: 6 November 2000 / Published online: 9 February 2001     

Review of ultrafast spectroscopy studies of valley carrier dynamics in two-dimensional semiconducting transition metal dichalcogenides

The two-dimensional layered transition metal dichalcogenides provide new opportunities in future valley-based information processing and also provide an ideal platform to study excitonic effects. At the center of various device physics toward their possible electronic and optoelectronic applications is understanding the dynamical evolution of various manyparticle electronic states, especially exciton which dominates the optoelectronic response of TMDs, under the novel context of valley degree of freedom. Here, we provide a brief review of experimental advances in using helicity-resolved ultrafast spectroscopy, especially ultrafast pump–probe spectroscopy, to study the dynamical evolution of valley-related many-particle electronic states in semiconducting monolayer transitional metal dichalcogenides.     

Dynamics of excimer laser ablation of thin tungsten films monitored by ultrafast photography

The time course of laser light induced transport of tungsten films from a glass support is followed by ultrafast photography using delayed dye laser pulses. The photographs provide unambiguous evidence that the material transport in the 40–200 mJ/cm² intensity domain takes place via removal of solid pieces from the film material. These results are consistent with heat flow calculations which predict the overall melting of the metal layer above 380 mJ/cm². The series of photographs presented give detailed insight into the melting process and have revealed an unexpected in-flight phase separation of solid fracture pieces and molten droplets throughout the 200–900 mJ/cm² domain. The faster propagating molten droplets form a condensed halo in front of the solid pieces, thereby providing an efficient shield between the processing laser light and the solid phase.     

Laser ablation of silicon and copper targets. Experimental and finite elements studies

The ablation process induced by excimer lasers is a collective phenomenon that basically involves two phenomena: the laser radiation–matter interaction and the dynamic of the ablation plume. The laser parameters, the thermal and optical properties of the material, and the surface morphology are critical factors in the ablation mechanisms affecting the direction of the ablation plume expansion. In this study, the role of the surface roughness and the evolution of its morphology under the laser irradiation were investigated. Assuming a thermal ablation model, a theoretical study of the initial steps of the laser ablation process by a finite element method using ANSYS (6.1) was performed. Different ablation experiments were carried out on silicon and copper targets using a XeCl laser. The target surface morphology changes were observed by SEM and the plume deflection was recorded by a digital camera. An acceptable agreement between the experimental and simulated results was found. This study contributes to a better understanding of the physical processes involved in the laser ablation and the relations between the plume deflection angle and the surface roughness. PACS 79.20.Ds; 81.40.Gh; 44.05.+e     

Ion dynamics in ultrafast laser ablation of copper target

We investigate the angular distribution and average kinetic energy of ions produced during ultrafast laser ablation （ULA） of a copper target in high vacuum. Laser produced plasma （LPP） is induced by irradiating the target with Ti：Sapphire laser pulses of -50 fs and 800 nm at an angle of incidence of 45°. An ion probe is moved along a circular path around the ablation spot, thereby allowing characterization of the time-of-flight （TOF） of ions at different angles relative to the normal target. The angular distribution of the ion flux is well-described by an adiabatic and isentropic expansion model of a plume produced by solid-target laser ablation （LA）. The angular width of the ion flux becomes narrower with increasing laser fluence. Moreover, the ion average kinetic energy is forward-peaked and shows a stronger dependence on the laser pulse fluence than on the ion flux. Such results can be ascribed to space charge effects that occur during the early stages of LPP formation.     

Solid phase formation of silicon nanocrystals by bulk ultrafast laser-matter interaction

Ultrashort pulse laser interaction with silica-silicon interfaces is presented as a means for all-solid-phase formation of high-purity silicon nanoparticles in the absence of ablation plumes or any substrate intermixing with surfaces in ambient air. Transmission electron microscopy and Raman spectroscopy provide definitive evidence for creation of nanocrystals in the silica host, while compressive stress in the silicon substrate corroborates the formation of optical waveguides parallel to the tracks.     

Experimental studies of phase transitions in isolated metal clusters

The reactions of isolated, neutral transition metal clusters with small molecules are used to probe cluster structure and to identify changes in structure with cluster size. Examples are presented of reactivity, adsorbate uptake, and product composition studies. The general conclusion is that transition metal clusters seem to have structure (are “solid”) under typical experimental conditions, and that their structure, i.e., the way the atoms pack, can change many times in the growth sequence from small clusters to bulk metal. These phase changes are often accompanied by dramatic changes in both chemical and physical properties. Evidence is presented for the existence of isomers of certain cluster sizes for some metals. In a few cases, the chemical evidence can be used to propose possible cluster structure; this is illustrated for iron and nickel clusters.     

Theoretical exploration of ultrafast spectroscopy of small clusters

We present the ultrafast multistate nuclear dynamics involving adiabatic and nonadiabatic excited states of non-stoichiometric halide deficient clusters (Na_nF_n-1) characterized by strong ionic bonding and one-excess electron for which the “frozen ionic bonds” approximation has been justified allowing to consider the optical response of the single excess electron in the effective field of the other electrons. We combined the Wigner-Moyal representation of the vibronic density matrix with the ab initio multi state molecular dynamics in the ground and excited electronic states including the nonadiabatic couplings calculated “on the fly” at low computational demand. This method allows the simulation of femtosecond pump-probe and pump-dump signals based on an analytical formulation, which utilizes temperature dependent ground state initial conditions, an ensemble of trajectories carried out on the electronic excited state as well as on the ground state after the passage through the conical intersection in the case of nonadiabatic dynamics and for probing either in the cationic state or in the ground state. The choice of the systems we presented has been made in order to determine the timescales of the fast geometric relaxation leaving the bonding frame intact as during the dynamics in the first excited state of Na₄F₃, and of the bond breaking processes leading to conical intersection between the first excited state and the ground state as in Na₃F₂. The former is the smallest finite system prototype for an surface F-center of bulk color centers. The latter allows to study the photo isomerization in full complexity taking into account all degrees of freedom. In the case of Na₄F₃ after the fast geometric relaxation in the excited state leading to deformed cuboidal structure without breaking of bonds, different types of internal vibrational redistribution (IVR) processes have been identified in pump-dump signals by tuning the dump laser. In contrast, from the analysis of the pump-probe signals of Na₃F₂ cluster, the timescales for the metallic and the ionic bond breaking, as well as for the passage through conical intersection have been determined. Finally the conditions under which these processes can be experimentally observed have been identified. Received 22 December 2000     

Studies of craters’ dimension for long-pulse laser ablation of metal targets at various experimental conditions

Long pulse laser shots of the PALS iodine laser in Prague have been used to obtain metal target ablation at various experimental conditions. Attention is paid mainly to the dependencies of the crater diameter on the position of minimum laser-focus spot with regard to the target surface, by using different laser wavelengths and laser energies. Not only a single one, but two minima, independently of the wavelength, of the target irradiation angle and of the target material, were recorded. Significant asymmetries, ascribed to the non-linear effects of intense laser beam with pre-formed plasma, were found, too. Estimations of ejected mass per laser pulse are reported and used to calculate the efficiency of laser-driven loading. Results on metal target ablation and crater formation at high intensities (from 2 × 10¹³ to 3 × 10¹⁶ W/cm²) are presented and compared. Crater depth, crater diameter and etching yield are reported versus the laser energy, in order to evaluate the ablation threshold fluence.     

高温合金不同脉宽超快激光作用下多脉冲去除阈值

实验研究了激光脉冲宽度和脉冲个数对镍基高温合金材料去除阈值的影响,分别在290 fs,1 ps和7 ps脉宽的激光下,使用1,10,50,100,300,500和1000个不同能量的激光脉冲辐照高温合金样品表面。实验结果表明,烧蚀坑尺寸会随脉冲数的增加而增加,而脉冲宽度的增加会加大脉冲个数对烧蚀坑直径的影响。通过烧蚀坑直径的平方值与激光脉冲能量之间存在的对数关系,得到了不同脉冲宽度下镍基高温合金的多脉冲材料阈值。3种不同脉宽下的高温合金多脉冲去除阈值都存在显著的累积效应。根据去除阈值计算得到290 fs,1 ps和7 ps脉宽下的累积效应系数分别为0.88,0.86和0.78。     

A model of laser ablation with temperature-dependent material properties,vaporization, phase explosion and plasma shielding

Laser ablation of metals using nanosecond pulses occurs mainly due to vaporization. However, at high fluences, when the target is heated close to its critical temperature, phase explosion also occurs due to homogeneous nucleation. Due to a wide variation in target temperature, the material properties also show a considerable variation. In this paper, a model of laser ablation is presented that considers vaporization and phase explosion as mechanisms of material removal and also accounts for the variation in material properties up to critical temperature using some general and empirical theories. In addition, plasma shielding due to inverse bremsstrahlung and photo-ionization is considered. The model predicts accurately (within 5 %) the phase explosion threshold fluence of Al. The predictions of ablation depth by the model are in reasonable agreement with experimental measurements at low fluences. Whereas, the degree of error marginally increases at high laser fluences.