Title: First-principles molecular dynamics simulations of the interaction of ionic projectiles with liquid water and ice
Author(s): Kohanoff J., Artacho E.
5th International Conference on Radiation Damage in Biomolecular Systems (Debrecen, Hyngary, 2008), AIP Conference Proceedings, 1080, pp. 78-87 (JUN 13-15 2008)Abstract
We first present results of first-principles molecular dynamics simulations of the passage of Carbon projectiles through water in the liquid state in the adiabatic regime, where the electrons are always in the instantaneous ground state. We study a range of projectile velocities up to the estimated upper limit for the adiabatic approximation and analyze the different types of collision events. We show that for high projectile velocities collisions are mostly binary, but at lower velocities most trajectories exhibit a continuous energy loss to the medium.. which cannot be properly described as a sequence of independent binary collisions. For the slowest projectiles we observe the formation of new chemical species such as hydronium, H5O2+ and hydrogen peroxide. When C-atoms are completely stopped, then we also see the formation of species like formic acid. By analyzing the generation of secondary fragments, we observe that these are mostly hyperthermal and their spatial rate of generation increases with decreasing projectile energy. The two most numerous species are H and OH. In the second part we study., via electronic dynamics with fixed nuclei, the opposite regime of very fast protons producing only electronic excitation in ice, under channeling conditions. We observe the existence of a threshold velocity for electronic excitation of about 0.2 a.u. By monitoring the rate of increase of the total energy, we calculate the electronic stopping power.
Title: Compton scatter profiles for warm dense matter
Author(s): Sahoo S., Gribakin G.F., Naz G.S., Kohanoff J., Riley D.,
Physical Review E, 77, No. 4 (2008)
In this paper, we discuss the possibility of using x-ray Compton scattering as a probe of the outer electronic structure of ions immersed in warm dense matter. It is proposed that the x-ray free-electron lasers currently under construction will provide an ideal tool for this, with the main pulse being used to create a uniform well-defined sample and the third harmonic providing a clean monochromatic probe. We model the plasma photon scatter spectrum by combining self-consistent finite-temperature electronic structure calculations with molecular dynamics simulations of the ion-ion structure factor. In particular, we present bound-free Compton profiles that are more accurate that those obtained using form factor or impulse approximations.
Title: Effect of quantization of vibrations on the structural properties of crystals
Author(s): Scivetti I., Gidopoulos N., Kohanoff J.,
Physical Review B, 78, No. 22 (2008)
We study the structural effects produced by the quantization of vibrational degrees of freedom in periodic crystals at zero temperature. To this end we introduce a methodology based on mapping a suitable subspace of the vibrational manifold and solving the Schrodinger equation in it. A number of increasingly accurate approximations ranging from the quasiharmonic approximation (QHA) to the vibrational self-consistent field (VSCF) method and the exact solution are described. A thorough analysis of the approximations is presented for model monatomic and hydrogen-bonded chains, and results are presented for a linear H-F chain where the potential-energy surface is obtained via first-principles electronic structure calculations. We focus on quantum nuclear effects on the lattice constant and show that the VSCF is an excellent approximation, meaning that correlation between modes is not extremely important. The QHA is excellent for covalently bonded mildly anharmonic systems, but it fails for hydrogen-bonded ones. In the latter, the zero-point energy exhibits a nonanalytic behavior at the lattice constant where the H atoms center, which leads to a spurious secondary minimum in the quantum-corrected energy curve. An inexpensive anharmonic approximation of noninteracting modes appears to produce rather good results for hydrogen-bonded chains for small system sizes. However, it converges to the incorrect QHA results for increasing size. Isotope effects are studied for the first-principles H-F chain. We show how the lattice constant and the H-F distance increase with decreasing mass and how the QHA proves to be insufficient to reproduce this behavior.
Title: Evidence of short-range screening in shock-compressed aluminum plasma
Author(s): Saiz E.G., Gregori G., Khattak F.Y., Kohanoff J., Sahoo S., Naz G.S., Bandyopadhyay S., Notley M., Weber R.L., Riley D.,
Physical Review Letters, 101, No. 7 (2008)
We have investigated the angular variation in elastic x-ray scattering from a dense, laser-shock-compressed aluminum foil. A comparison of the experiment with simulations using an embedded atom potential in a molecular dynamics simulation shows a significantly better agreement than simulations based on an unscreened one-component plasma model. These data illustrate, experimentally, the importance of screening for the dense plasma static structure factor.