M.J. Caturla

Comparative study of radiation damage accumulation in Cu and Fe

Bcc and fcc metals exhibit significant differences in behavior when exposed to neutron or heavy ion irradiation. Transmission electron microscopy (TEM) observations reveal that damage in the form of stacking fault tetrahedra (SFT) is visible in copper irradiated to very low doses, but that no damage is visible in iron irradiated to the same total dose. In order to understand and quantify this difference in behavior, we have simulated damage production and accumulation in fcc Cu and bcc Fe. We use 20 keV primary knock-on atoms (PKAs) at a homologous temperature of 0.25 of the melting point. The primary damage state was calculated using molecular dynamics (MD) with empirical, embedded-atom interatomic potentials. Damage accumulation was modeled using a kinetic Monte Carlo (kMC) algorithm to follow the evolution of all defects produced in the cascades. The diffusivities and binding energies of defects are input data for this simulation and were either extracted from experiments, the literature, or calculated using MD. MD simulations reveal that vacancy clusters are produced within the cascade core in the case of copper. In iron, most of the vacancies do not cluster during cooling of the cascade core and are available for diffusion. In addition, self-interstitial atom (SIA) clusters are produced in copper cascades but those observed in iron are smaller in number and size. The combined MD/kMC simulations reveal that the visible cluster densities obtained as a function of dose are at least one order of magnitude lower in Fe than in Cu. We compare the results with experimental measurements of cluster density and find excellent agreement between the simulations and experiments when small interstitial clusters are considered to be mobile as suggested by recent MD simulations.

Ab initio energetics of boron-interstitial clusters in crystalline Si

We have performed an extensive first-principles study of the energetics of boron clustering in silicon in the presence of excess self-interstitial atoms (SIAs). We consider complexes with up to four B atoms and two SIAs. We have conducted an extensive search for the ground-state configurations and charge states of these clusters. We find the cluster containing three B atoms and one SIA(B3I) to be remarkably stable, while all our clusters with more than 80% boron content are unstable. Hence, we propose B3I to be a stable nucleus that can grow to larger clusters. The energetics presented here can be used as input to large-scale predictive models for B diffusion and activation during ion implantation and thermal annealing.

Disordering and defect production in silicon by keV ion irradiation studied by molecular dynamics

Abstract We discuss the use of molecular dynamics simulation methods to study disordering and ion implantation in silicon. We discuss the simulation methodology and introduce the interatomic potential employed, with a critical discussion of its applicability. We show that in silicon the displacement cascade results in a distinct primary state of damage dominated by large pockets of highly unrelaxed amorphous-like disordered silicon. The amorphous volume produced for 5 keV Si on Si cascades contains ≈ 1000 atoms, corresponding to an energy cost of approximately 10 eV/atom. Replacement collision sequences are found to be very short in silicon and as a result, very few point defects appear as a consequence of the displacement cascade. We show that upon annealing of the damage microstructure at high temperature, the amorphous pockets recrystallize and result in the freezing-in in the lattice of vacancies, SIAs and their clusters. We discuss the effect of the ion mass on defect production and amorphization, and present results on the temperature dependence of the damage as well on the stability of the damage clusters for boron and arsenic cascades.

Densification of fused silica due to shock waves and its implications for 351 nm laser induced damage.

High-power 351 nm (3 ) laser pulses can produce damaged areas in high quality fused silica optics. Recent experiments have shown the presence of a densified layer at the bottom of damage initiation craters. We have studied the propagation of shock waves through fused silica using large-scale atomistic simulations since such shocks are expected to accompany laser energy deposition. These simulations show that the shocks induce structural transformations in the material that persist long after the shock has dissipated. Values of densification and thickness of densified layer agree with experimental observations. Moreover, our simulations give an atomistic description of the structural changes in the material due to shock waves and their relation to Raman spectra measurements.

Mechanical property degradation in irradiated materials: A multiscale modeling approach

Abstract High-energy particle irradiation of low stacking fault energy, face centered cubic (fcc) metals produces significant degradation of mechanical properties, as evidenced in tensile tests performed at or near room temperature. Post-irradiation microstructural examination reveals that approximately 90% of the radiation-induced defects in copper are stacking fault tetrahedra (SFT). Radiation damage is an inherently multiscale phenomenon involving processes spanning a wide range of length and time scales. Here we present a multiscale modeling methodology to study the formation and evolution of defect microstructure and the corresponding mechanical property changes under irradiation. At the atomic scale, molecular dynamics (MD) simulations have been used to study the evolution of high energy displacement cascades, SFT formation from vacancy rich regions of displacement cascades, and the interaction of SFTs with moving dislocations. Defect accumulation under irradiation is modeled over diffusional length and time scales by kinetic Monte Carlo (KMC), utilizing a database of displacement cascades generated by MD. The mechanical property changes of the irradiated material are modeled using three-dimensional dislocation dynamics (DD). Key input into the DD includes the spatial distribution of defects produced under irradiation, obtained from KMC, and the fate of dislocation interactions with SFTs, obtained from MD.

Large enhancement of boron solubility in silicon due to biaxial stress

One of the important challenges to the semiconductor industry today is to enhance the solid solubility of several dopants, boron in particular, in silicon. We calculate the equilibrium solid solubility of boron in Si from first principles and examine the effect of biaxial stress. We find an unexpectedly large enhancement, on the order of 150%, for only 1% strain primarily due to the charge of the substitutional boron impurity in Si. We point out that this effect is an intrinsic property of Si and is expected to be important for other dopants as well.

A kinetic Monte-Carlo study of the effective diffusivity of the silicon self- interstitial in the presence of carbon and boron

The effect of carbon on self-interstitial diffusion in Si is studied by means of a kinetic Monte–Carlo simulation. It is found that modest levels of carbon (≳1017 cm−3) significantly reduce the effective interstitial diffusivity. From fitting self-interstitial profiles, migration energies and prefactors of the effective diffusivity have been determined for a variety of background carbon levels. In addition, we re-examine recent experiments performed in samples with significant levels of carbon, which attempt to measure the effective diffusivity by monitoring the spreading of boron marker layers. We show that the presence of boron in delta-doped markers significantly alters the measured self-interstitial diffusivity.

Atomic scale models of ion implantation and dopant diffusion in silicon

We review our recent work on an atomistic approach to the development of predictive process simulation tools. First-principles methods, molecular dynamics simulations, and experimental results are used to construct a database of defect and dopant energetics in Si. This is used as input for kinetic Monte Carlo simulations. C and B trapping of the Si self-interstitial is shown to help explain the enormous disparity in its measured diffusivity. Excellent agreement is found between experiments and simulations of transient enhanced diffusion following 20‐80 keV B implants into Si, and with those of 50 keV Si implants into complex B-doped structures. Our simulations predict novel behavior of the time evolution of the electrically active B fraction during annealing. q 2000 Published by Elsevier Science S.A. All rights reserved.

Defect production and annealing kinetics in elemental metals and semiconductors

Abstract We present a review of recent results of molecular dynamics (MD) and kinetic Monte Carlo (KMC) simulations of defect production and annealing in irradiated metals and semiconductors. The MD simulations describe the primary damage state in elemental metals Fe, V and Au, and in an elemental semiconductor Si. We describe the production of interstitial and vacancy clusters in the cascades and highlight the differences among the various materials. In particular, we discuss how covalent bonding in Si affects defect production and amorphization resulting in a very different primary damage state from the metals. We also use MD simulations to extract prefactors and activation energies for migration of point defects, as well as to investigate the energetics, geometry and diffusivity of small vacancy and interstitial clusters. We show that, in the metals, small interstitial clusters are highly mobile and glide in one dimension along the direction of the Burgers vector. In silicon, we show that, in contrast to the metals, the neutral vacancy diffuses faster than the neutral self-interstitial. The results for the primary damage state and for the defect energetics and kinetics are then combined and used in a kinetic Monte Carlo simulation to investigate the escape efficiency of defects from their nascent cascade in metals, and the effect of dose rate on damage accumulation and amorphization in silicon. We show that in fee metals Au and Pb at or above stage V the escape probability is approximately 40% for 30 keV recoils so that the freely migrating defect fraction is approximately 10% of the dpa standard. In silicon, we show that damage accumulation at room temperature during light ion implantation can be significantly reduced by decreasing the dose rate. The results are compared to scanning tunneling microscopy experiments.

Simulation of damage production and accumulation in vanadium

Energetic atoms which have been knocked-off their lattice sites by neutron or ion irradiation leave a trail of vacancies and interstitials in their wake. Most of these defects recombine with their opposites within their own collision cascade. Some fraction, however, escape to become freely migrating defects (FMD) in the bulk of the material. The interaction of FMD with the microstructure has long been linked to changes in the macroscopic properties of materials under irradiation. We calculate the fraction of FMD in pure vanadium for a wide range of temperatures and primary knock-on atom (PKA) energies. The collision cascade database is obtained from molecular dynamics (MD) simulations with an embedded atom method (EAM) potential. The actual FMD calculation is carried out by a kinetic Monte Carlo (kMC) code with a set of parameters extracted either from the experimental literature or from MD simulations. Annealing each individual cascade at different temperatures allows the mobile species to escape and account for FMD. We also analyze damage accumulation in a specimen irradiated at low dose rate in the presence of impurities. At the temperature studied, beginning of stage V, we observe that only vacancies are free to move whereas most interstitials are stopped by impurities. We also analyze the role of impurities on damage accumulation and on the concentration of mobile defects.