No abstract available

[en] Fast moving ions travel great distances along channels between low-index crystallographic planes, slowing through collisions with electrons, until finally they hit a host atom initiating a cascade of atomic displacements. Statistical penetration ranges of incident particles are reliably used in ion-implantation technologies, but a full, necessarily quantum-mechanical, description of the stopping of slow, heavy ions is challenging and the results of experimental investigations are not fully understood. Using a self-consistent model of the electronic structure of a metal, and explicit treatment of atomic structure, we find by direct simulation a resonant accumulation of charge on a channelling ion analogous to the Okorokov effect but originating in electronic excitation between delocalized and localized valence states on the channelling ion and its transient host neighbours, stimulated by the time-periodic potential experienced by the channelling ion. The charge resonance reduces the electronic stopping power on the channelling ion. These are surprising and interesting new chemical aspects of channelling, which cannot be predicted within the standard framework of ions travelling through homogeneous electron gases or by considering either ion or target in isolation. (paper)

[en] We present an investigation of systematic trends for the self-interstitial atom (SIA) defect behavior in body-centered cubic (bcc) transition metals using density-functional calculations. In all the nonmagnetic bcc metals the most stable SIA defect configuration has the <111> symmetry. Metals in group 5B of the periodic table (V, Nb, Ta) have significantly different energies of formation of the <111> and <110> SIA configurations, while for the group 6B metals (Cr, Mo, W) the two configurations are linked by a soft bending mode. The relative energies of SIA defects in the nonmagnetic bcc metals are fundamentally different from those in ferromagnetic bcc α-Fe. The systematic trend exhibited by the SIA defect structures in groups 5B and 6B transition metals correlates with the observed thermally activated mobility of SIA defects

[en] Atomistic simulations are a primary means of understanding the damage done to metallic materials by high energy particulate radiation. In many situations the electrons in a target material are known to exert a strong influence on the rate and type of damage. The dynamic exchange of energy between electrons and ions can act to damp the ionic motion, to inhibit the production of defects or to quench in damage, depending on the situation. Finding ways to incorporate these electronic effects into atomistic simulations of radiation damage is a topic of current major interest, driven by materials science challenges in diverse areas such as energy production and device manufacture. In this review, we discuss the range of approaches that have been used to tackle these challenges. We compare augmented classical models of various kinds and consider recent work applying semi-classical techniques to allow the explicit incorporation of quantum mechanical electrons within atomistic simulations of radiation damage. We also outline the body of theoretical work on stopping power and electron-phonon coupling used to inform efforts to incorporate electronic effects in atomistic simulations and to evaluate their performance.

[en] By simulating the passage of heavy ions along open channels in a model crystalline metal using semi-classical Ehrenfest dynamics we directly investigate the nature of non-adiabatic electronic effects. Our time-dependent tight-binding approach incorporates both an explicit quantum mechanical electronic system and an explicit representation of a set of classical ions. The coupled evolution of the ions and electrons allows us to explore phenomena that lie beyond the approximations made in classical molecular dynamics simulations and in theories of electronic stopping. We report a velocity-dependent charge-localization phenomenon not predicted by previous theoretical treatments of channelling. This charge localization can be attributed to the excitation of electrons into defect states highly localized on the channelling ion. These modes of excitation only become active when the frequency at which the channelling ion moves from interstitial point to equivalent interstitial point matches the frequency corresponding to excitations from the Fermi level into the localized states. Examining the stopping force exerted on the channelling ion by the electronic system, we find broad agreement with theories of slow ion stopping (a stopping force proportional to velocity) for a low velocity channelling ion (up to about 0.5 nm fs⁻¹ from our calculations), and a reduction in stopping power attributable to the charge localization effect at higher velocities. By exploiting the simplicity of our electronic structure model we are able to illuminate the physics behind the excitation processes that we observe and present an intuitive picture of electronic stopping from a real-space, chemical perspective. (paper)

[en] The solution of the time-dependent Schroedinger equation for systems of interacting electrons is generally a prohibitive task, for which approximate methods are necessary. Popular approaches, such as the time-dependent Hartree-Fock (TDHF) approximation and time-dependent density functional theory (TDDFT), are essentially single-configurational schemes. TDHF is by construction incapable of fully accounting for the excited character of the electronic states involved in many physical processes of interest; TDDFT, although exact in principle, is limited by the currently available exchange-correlation functionals. On the other hand, multiconfigurational methods, such as the multiconfigurational time-dependent Hartree-Fock (MCTDHF) approach, provide an accurate description of the excited states and can be systematically improved. However, the computational cost becomes prohibitive as the number of degrees of freedom increases, and thus, at present, the MCTDHF method is only practical for few-electron systems. In this work, we propose an alternative approach which effectively establishes a compromise between efficiency and accuracy, by retaining the smallest possible number of configurations that catches the essential features of the electronic wavefunction. Based on a time-dependent variational principle, we derive the MCTDHF working equation for a multiconfigurational expansion with fixed coefficients and specialise to the case of general open-shell states, which are relevant for many physical processes of interest.

[en] In this review we consider those processes in condensed matter that involve the irreversible flow of energy between electrons and nuclei that follows from a system being taken out of equilibrium. We survey some of the more important experimental phenomena associated with these processes, followed by a number of theoretical techniques for studying them. The techniques considered are those that can be applied to systems containing many non-equivalent atoms. They include both perturbative approaches (Fermi's Golden Rule and non-equilibrium Green's functions) and molecular dynamics based (the Ehrenfest approximation, surface hopping, semi-classical Gaussian wavefunction methods and correlated electron-ion dynamics). These methods are described and characterized, with indications of their relative merits