Stochastic void coarsening

The random nature of diffusing jumps and cascade occurrence produce stochastic fluctuations of the point-defect fluxes. The effect of such fluctuations on the kinetics of void growth is investigated in the present paper. It is found that the non-linear coupling between the stochastic fluctuations and the void sizes may lead to the instability of void evolution within the mean-field theory, when the sizes of voids and their growth rates are both relatively small. The growth rate of voids becomes dominated by the stochastic component, causing the smaller voids to shrink away. This effect is investigated in terms of a non-equilibrium phase transition induced by a purely random stochastic noise. The derived conditions for this non-equilibrium transition are compared favourably with experimental observations. Received: 5 June 2000 / Accepted: 9 October 2000 / Published online: 21 March 2001     

The stability of homogeneous microstructure development under cascade-damage conditions

The development of microstructure, under cascade-damage conditions, in regions far away from any major sink is considered. Within the mean-field theory, a homogeneous distribution of point defects and their clusters is a pre-imposed artificial constraint on the kinetic system. The resulting excessive recombination of the vacancies and interstitials at a high density of accumulated point-defect clusters dictates a low rate of void growth. Considerations beyond the mean-field theory, by taking into account the concentration fluctuations of both the point defects and their clusters, relax the restriction of the homogeneous distribution. In this paper, we consider a system without pre-existing sinks, except the void nuclei, in which vacancies, interstitials and their clusters are continuously produced. Taking into account the mobility of small clusters and the stochastic fluctuations of the point-defect fluxes, a kinetic theory is formulated from first principles. It is rigorously shown that through the stochastic fluctuations, and the positive-feedback action of the mobility of the small clusters on the interstitial concentration, the homogeneous interstitial distribution is unstable at temperatures above stage V, leading to the formation of a spatially heterogeneous microstructure in pure metals at low irradiation doses. The characteristics of the microstructure evolution and void swelling, predicted from the theory, are found to be in good agreement with the experimental results. Received: 17 March 2000 / Accepted: 17 October 2000 / Published online: 25 July 2001     

Diffusion anisotropy and void development under cascade irradiation

Cascade irradiation of metals gives rise to swelling as a result of the creation of voids and the evolution of the void ensemble. Under suitable circumstances, the originally disordered void distribution transforms into to a void lattice. As demonstrated previously, the understanding of the evolution and the unique features of the void ensemble requires a difference in the anisotropy of the diffusion (DAD) of vacancies and self-interstitial atoms (SIAs), which is achieved by one-dimensional diffusion of the SIAs. On the other hand, void swelling has been successfully modeled in terms of three-dimensional diffusion of both vacancies and SIAs. In the present paper it is shown that these seemingly contradicting interpretations and all related observations can be quantitatively reconciled by a small DAD created by only ～1% of SIAs diffusing one-dimensionally. It is also demonstrated that at the initial stage of void-lattice formation, ordering occurs mainly on close-packed crystal planes, which is in contrast to the naïve expectation that one-dimensional diffusion of SIAs should result in a void ordering along close-packed directions. Finally it is found that, in the case of a small DAD, voids annihilate via stochastic shrinkage much faster than by coalescence. This falsifies the argument in the literature that one-dimensional diffusion of SIAs would necessarily lead to the coalescence of voids and destabilization of the void lattice.     

Void ordering in hexagonal close-packed metals

Voids occur in solids exposed to high-temperature particle irradiation. In hexagonal metals with lattice-parameter ratiosc/a which are smaller than for ideal close-packing, voids arranged in layers parallel to the basal plane have been observed after high-dose irradiation, whereas more perfect void ordering, e.g. the formation of void lattices like in cubic metals, has not been found. In this paper it is shown that it is the two-dimensional diffusion of self-interstitial atoms in the basal plane which gives rise to the layer-type arrangement of voids. The possibility of other void-ordering phenomena in hexagonal metals is investigated. It is demonstrated that, under certain circumstances, one-dimensional diffusion of a metastable self-interstitial configuration may lead to the arrangement of voids in columns perpendicular to the basal plane.     

Surface morphology of MgO (100) crystals implanted with MeV Al+ and Al2+ ions

MgO (100) single crystals are implanted with 1.50-MeV Al⁺ and 3.00-MeV Al₂ ⁺ ions at a fluence of 1×10¹⁵ Al  atoms  cm^-2 under high-vacuum conditions. The surface morphology of the substrate is measured in air using atomic force microscopy and X-ray reflectometry followed by computer-simulated spectrum analysis. The ion-irradiated areas are found to protrude to different heights on the nanometre scale. Small height differences are observed in the areas irradiated by Al⁺ and Al₂ ⁺ ions of comparable energy, dose rate and total fluence. The results indicate that protrusions are most likely caused by implantation-induced point defects (vacancies) generated in the crystal during implantation. Other possibilities for the cause of protrusions are discussed. Thermal treatment stimulates a partial recovery of the implantation damage and alters the topography of MgO surfaces. Received: 22 May 2001 / Accepted: 30 May 2001 / Published online: 25 July 2001     

Ultrashort-laser-pulse-driven rewritable phase-change optical recording in Sb-based films

This paper reviews the work we have carried out over the last years on the development of ultrashort-laser-pulse-driven, rewritable, phase-change optical memories. The materials we have tailored for this application are non-stoichiometric, Sb-rich amorphous thin films, which can be crystallized upon irradiation with ultrashort laser pulses, showing a large optical contrast upon transformation. This result makes them very promising for the development of rewritable phase-change optical memories under ultrashort pulses, since the reversibility of the process has also been demonstrated. Adequate control of the heat-flow conditions has allowed us to achieve a full transformation time faster than 400 ps for crystallization/amorphization using 30-ps pulses. The crystallization threshold fluence has been found to decrease upon irradiation with pulses shorter than 800 fs, thus suggesting the relevance of high-electronic-excitation-induced processes in the amorphous-to-crystalline phase transition. This has been confirmed by the observation of an ultrafast, non-thermal phase transition occurring 200–300 fs after the arrival of the laser pulse at the surface, for fluences above the crystallization threshold. The presence of this transient phase conditions the final state induced therefore enabling the applicability of this material as a rewritable recording medium using femtosecond pulses. Received: 11 October 2001 / Accepted: 9 July 2002 / Published online: 25 October 2002 RID="*" ID="*"Corresponding author. Fax: +34-91/564-5557, E-mail: J.Solis@io.cfmac.csic.es     

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     

On the migration of defects and impurities in microelectromechanical systems subject to a large number of light pulses

The migration of defects in light-irradiated microelectromechanical systems (MEMS) is treated theoretically. The effects of temperature gradients on atomic demixing are considered. It is found that, when the migration energy of defects and impurities is less than about 0.5 eV, their migration has to be introduced in the modelling of ageing of MEMS. Received: 17 July 2000 / Accepted: 31 March 2000 / Published online: 27 June 2001     

Femtosecond laser‐assisted formation of channels in sapphire using KOH solution

We report on wet etching of photomodified regions in crystalline sapphire using KOH solution. Tightly focused femtosecond laser pulses (150 fs at 800 nm wavelength) were used to create void structures enclosed in an amorphised sapphire shell inside the bulk of a crystalline host. The diameter of the amorphous regions can be controlled by pulse energy and was typically 0.5–1.5 µm. The etching rate depends on the distance between adjacent irradiation spots, pulse energy, concentration of etchant and ultrasonic agitation.

     

Dynamics of the plume formation and parameters of the ejected clusters in short-pulse laser ablation

The dynamics of the early stages of the ablation plume formation and the mechanisms of cluster ejection are investigated in large-scale molecular dynamics simulations. The cluster composition of the ablation plume has a strong dependence on the irradiation conditions and is defined by the interplay of a number of processes during the ablation plume evolution. At sufficiently high laser fluences, the phase explosion of the overheated material leads to the formation of a foamy transient structure of interconnected liquid regions that subsequently decomposes into a mixture of liquid droplets, gas-phase molecules, and small clusters. The ejection of the largest droplets is attributed to the hydrodynamic motion in the vicinity of the melted surface, especially active in the regime of stress confinement. Spatially resolved analysis of the dynamics of the plume formation reveals the effect of segregation of the clusters of different sizes in the expanding plume. A relatively low density of small/medium clusters is observed in the region adjacent to the surface, where large clusters are being formed. Medium-size clusters dominate in the middle of the plume and only small clusters and monomers are observed near the front of the expanding plume. Despite being ejected from deeper under the surface, the larger clusters in the plume have substantially higher internal temperatures as compared to the smaller clusters. The cluster-size distributions can be relatively well described by a power law Y(N)∼N^-τ with exponents different for small, up to ∼15 molecules, and large clusters. The decay is much slower in the high-mass region of the distribution. Received: 13 October 2001 / Accepted: 18 July 2002 / Published online: 25 October 2002 RID="*" ID="*"Corresponding author. Fax: +1-434/982-5660, E-mail: lz2n@virginia.edu     

Ion synthesis and laser annealing of Cu nanoparticles in Al2O3

Al₂O₃ samples with Cu nanoparticles, synthesised by ion implantation at 40 keV with a dose of 1×10¹⁷ ion/cm² and a current density from 2.5 to 12.5 μA/cm², were annealed using ten pulses from a KrF excimer laser with a single pulse fluence of 0.3 J/cm². The copper depth distribution, formation and modification of metal nanoparticles under the ion implantation and laser treatment were studied by Rutherford backscattering (RBS), energy dispersive X-ray (EDX) analysis, atomic force microscopy (AFM) and optical spectroscopy. It was found that laser annealing leads to a reduction in the nanoparticle size without diffusion of metal atoms into the bulk. The change in particle size and the possibility for oxidation of the copper particles are examined in the framework of Mie theory. Calculations presented show that under excimer laser treatment, Cu nanoparticles are more likely to be reduced in size than to undergo oxidation. Received: 19 April 2001 / Accepted: 7 November 2001 / Published online: 23 January 2002     

Effect of refractive index-mismatch on laser microfabrication in silica glass

We studied the peculiarities of femtosecond laser microfabrication in silica glass with a refractive index that did not exactly match the value for which the focusing optics is designed. Spherical aberrations resulting from a small refractive index mismatch were found to increase the size and distort the shape of photodamaged regions, thus reducing the spatial resolution of the microfabrication. However, these undesirable effects can be minimized, providing that the focusing depth inside the glass is not too large, and the laser intensity is kept close to the light-induced damage threshold. Received: 3 December 2001 / Accepted: 11 April 2002 / Published online: 10 September 2002 RID="*" ID="*"Corresponding author. Fax: +81-88/656-7598, E-mail: misawa@eco.tokushima-u.ac.jp     

Electric field of a buried interfacial region measured by positron-lifetime spectroscopy

Positrons from a radioactive source are implanted into a reverse-biased metal–semiconductor contact and are drifted back towards the contact by the internal electric field where they trap into voids and annihilate. The electric field dependent interface annihilation fraction is monitored by way of the intensity of the long (∼400–500 ps) void lifetime component using positron-lifetime spectroscopy. Unlike previous analyses of such systems a numerical model involving positron drift, annihilation and trapping into the interfacial state has been constructed to describe the positron dynamics in the presence of the non-uniform junction electric field. The use of the positron-lifetime technique in probing the internal electric field at buried contacts is thus demonstrated. Results obtained using the numerical method for the Au, Al and Ni/Semi-Insulating (SI)-GaAs contact systems are found to be consistent with the findings of previous studies on the Au/SI-GaAs system. Received: 29 November 2000 / Accepted: 26 February 2001 / Published online: 25 July 2001     

X-ray-induced photochromic effects in copper-doped lithium niobate crystals

X-Ray-induced absorption changes in Cu-doped lithium niobate crystals (LiNbO₃) are investigated. All induced photochromic effects are fully reversible, i.e., illumination with white light annihilates the absorption changes. With increasing doping level, a decrease in the saturation value of the absorption changes is found. Changes of the Li concentration of the crystal to a more stoichiometric composition via Li indiffusion further decreases the photochromic effect. For sufficient X-ray doses, the saturation value is independent of the radiation energy in the measured range from 50–150 kV. The spectral distribution of the X-ray-induced absorption changes and the slow dark decay indicate that the additional absorption results from an increase of the Cu⁺ concentration. Received: 20 December 2000 / Revised version: 24 January 2001 / Published online: 27 April 2001     

Structural and electrical characteristics of zirconium oxide layers derived by photo-assisted sol–gel processing

This paper reports the photo-assisted formation of ZrO₂ layers derived by sol–gel processing at low temperatures using intense radiation from ultraviolet (UV) excimer lamps. Excellent layer properties can be readily obtained for these sol–gel layers after 5-min exposure to the UV irradiation at around 300 °C. Analyses of the as-deposited sol–gel layers by UV/VIS spectrophotometry show that the organic species contained in the layers have been removed to a large extent after 5-min irradiation. This is further confirmed by X-ray photoelectron spectroscopy analyses of the same irradiated layers, which indicate the formation of ZrO₂ with little carbon contamination contributed by the organic species and less oxidation of Si at the interface. Electrical measurements of these layers are also reported. Received: 31 July 2001 / Accepted: 6 September 2001 / Published online: 17 October 2001     

Femtosecond ablation of ultrahard materials

Several ultrahard materials and coatings of definite interest for tribological applications were tested with respect to their response when irradiated with fs laser pulses. Results on cemented tungsten carbide and on titanium carbonitride are reported for the first time and compared with outcomes of investigations on diamond and titanium nitride. The experiments were carried out in air, in a regime of 5–8 J/cm² fluences, using the beam of a commercial Ti:sapphire laser. The changes induced in the surface morphology were analysed with a Nomarski optical microscope, and with SEM and AFM techniques. From the experimental data and from the calculated incident energy density distributions, the damage and ablation threshold values were determined. As expected, the diamond showed the highest threshold, while the cemented tungsten carbide exhibited typical values for metallic surfaces. The ablation rates determined (under the above-mentioned experimental conditions) were in the range 0.1–0.2 μm per pulse for all the materials investigated. Received: 31 August 2001 / Accepted: 3 December 2001 / Published online: 20 March 2002     

Comparative studies of absorptance behaviour of alkaline-earth fluorides at 193 nm and 157 nm

Absorptance losses in MgF₂, CaF₂ and BaF₂ during 193-nm (DUV) and 157-nm (VUV) irradiation are investigated by employing a high-resolution laser calorimetric technique which allows the determination of both single- and two-photon absorptance at energy densities up to 110 mJ/cm². A strong wavelength dependence of the DUV and VUV absorption characteristics is observed: while effective two-photon absorption takes place at 193 nm, either no similar effect at all (in the case of BaF₂) or only a very minor effect (CaF₂) is observed at 157 nm. A first explanation for this absorption behaviour is given, implying the energetic band structure of CaF₂. In addition it is shown that, due to the strong nonlinear dependency, above a critical energy density the absorptance at 193 nm can exceed the absorptance at 157 nm. Furthermore, different single- and two-photon absorption coefficients are determined for different CaF₂ samples at 193 nm, indicating a two-step absorption mechanism. In addition, laser-induced aging is found in a MgF₂ sample at 193 nm, but not at 157 nm. Received: 21 June 2001 / Revised version: 2 November 2001 / Published online: 7 February 2002     

Transmission electron microscopy studies of femtosecond laser induced modifications in quartz

Cross-sectional transmission electron microscopy investigations of femtosecond laser induced sub-micrometer structural modifications inside crystalline quartz were carried out. Modifications from single laser shots and from lines built of overlapping shots were imaged. Both single laser shot modifications and line structures show an amorphous core surrounded by a disturbed crystalline structure. A strong strain field surrounding the central, irradiated, core is responsible for an increase of the refractive index. Finite element method calculations of the strain field show maxima on both sides of the irradiated core, which are in good agreement with optical measurements of the refractive-index change. Received: 29 September 2001 / Accepted: 9 July 2002 / Published online: 25 October 2002 RID="*" ID="*"Corresponding author. Fax: +49-3641/947792, E-mail: tatiana.gorelik@rz.uni-jena.de     

γ-ray irradiation effect on hysteresis symmetry and data retention of Pt/SrBi2Ta2O9/Pt thin-film capacitors

The γ-ray irradiation effect on hysteresis symmetry and data retention of Pt/SrBi₂Ta₂O₉/Pt ferroelectric thin-film capacitors has been investigated as a function of irradiation dose. A horizontal shift of polarization–voltage curves along the voltage axis, known as imprint, was observed after the polarized capacitors had been irradiated. The voltage shift increased with increasing irradiation dose and increasing remanent polarization written before irradiation. After irradiation, severe data loss was observed after these capacitors had been written to the state opposite to the one stored during irradiation. Possible functional failure due to such a data loss was discussed. Received: 17 January 2001 / Revised version: 27 April 2001 / Published online: 20 June 2001