Elastic properties of compressed rare-gas crystals in a model of deformable atoms

Physics of the Solid State - The elastic properties of compressed Ne, Ar, Kr, and Xe rare-gas crystals were studied in a model of deformable and polarizable atoms. The second-order Fuchs elasticity...     

Lattice dynamics in heavy rare-gas crystals under pressure

The lattice dynamics of compressed rare-gas crystals is theoretically investigated within the ab initio approach in the framework of the Tolpygo model, which explicitly includes the deformation of electron shells in the dipole approximation. The phonon frequencies of compressed rare-gas crystals are calculated with allowance made for the electron-phonon interaction at the mean-value points with the use of the dynamic matrix constructed with the ab initio short-range repulsive potential. The energy of zero-point vibrations and the heat capacity of compressed krypton and xenon face-centered cubic crystals are calculated in the harmonic approximation. The calculated temperature dependences of the specific heat capacity and the Debye temperature are in good agreement with the data available in the literature on the experiment at zero pressure and the results of the calculations within the density-functional theory for all pressures. The quantum effects, in particular, the energies E _zp of zero-point vibrations for krypton and xenon crystals, are investigated at different pressures.     

Elastic properties of compressed crystalline Ne in the model of deformable atoms

An ab initio version of the model with deformable atoms has been constructed to investigate the elastic properties of compressed crystalline neon. Approximations for the calculating parameters of quadrupole deformation of atomic electron shells have been discussed. It has been shown that the pressure dependence of the deviation from the Cauchy relation δ is the result of two competitive interactions, namely, the many-body and electron-phonon interactions, which manifests itself in the deformation of atomic electron shells during the shift of nuclei. In the case of Ne, contributions of these interactions are compensated to a large degree, which provides a weakly pressure-dependent positive value for δ. The agreement of calculated elastic moduli and deviations from the Cauchy relation for Ne with the experiment is good.     

Lattice dynamics in light rare-gas crystals under pressure

The lattice dynamics of compressed neon and argon crystals has been theoretically investigated within the ab initio approach in the framework of the Tolpygo model, which explicitly includes the deformation of electron shells. The energy of zero-point vibrations, mean-square displacements, and specific heat capacities of compressed neon and argon face-centered cubic crystals have been calculated in the harmonic approximation using the dynamic matrix constructed with the ab initio short-range repulsive potential and integration over the mean-value points in the Brillouin zone. The calculated temperature dependences of the specific heat capacity and the Debye temperature are in good agreement with the data available in the literature on the experiment at zero pressure. The role of zero-point vibrations in the thermodynamics of the entire series of rare-gas crystals and, in particular, in the validity of the Lindemann melting criterion has been analyzed.     

Elastic constants of noble-gas crystals under pressure and the cauchy relations

Physics of the Solid State - The equations of state are solved and the elastic constants responsible for the propagation of sound in strongly compressed crystals of noble gases are calculated in...     

Optical absorption by rare-gas atoms in alkali-metal rare-gas alloys

We present results of a Cluster-Bethe Lattice Method calculation of the optical absorption due to rare-gasses in alkali-metal rare-gas alloys. A specific application to the Cs-Xe alloy reveals that the main features of the absorption for the whole concentration range can be understood in terms of a single-quasiparticle model. The effects of short-range order are investigated.     

Elastic properties of liquid crystals

The structural and elastic properties of 4-n′-pentyl-4′-cyanobiphenyl (5CB) in the nematic liquid-crystal phase are investigated in the framework of the statistical-mechanical theory and the molecular dynamics method.     

Elastic properties of layered crystals

The characteristic features of the elastic properties of layered crystals and their dependence on temperature and pressure are analyzed. The relations between the elastic constants of hexagonal layered crystals are given. It is shown that the anomalous behavior of the elastic constants in the temperature region of a phase transition affects both the magnitude and sign of the thermal expansion coefficients of layered crystals. From analyzing the pressure and temperature dependences of the elastic constants, it is found that the anharmonicity of the bonding forces between the layers is much greater than the anharmonicity of the intralayer forces. The contribution from thermal expansion to the variations of the elastic constants with temperature is estimated.     

Laser-enabled Auger decay in rare-gas atoms

In rare-gas atoms, Auger decay in which an inner-valence shell ns hole is filled is not energetically allowed. However, in the presence of a strong laser field, a new laser-enabled Auger decay channel can open up to increase the double-ionization yield. This process is efficient at high laser intensities, where an ns hole can be filled within a few femtoseconds of its creation. This novel laser-enabled Auger decay process is of fundamental importance for controlling electron dynamics in atoms, molecules, and materials.     

Experimental determination of the dynamical properties of molecular crystals under pressure

Abstract

A main characteristic of molecular solids is the large difference between intra- and intermolecular interactions. This difference is reflected in the physical properties, especially in the dynamical properties and their pressure dependence. The three main techniques used to study the dynamical properties of crystals in diamond cells are reviewed, and each one is illustrated by an example which shows specific properties of molecular crystals.     

Acceleration of atoms in crystals under plastic deformation

It is shown that a double-well potential can appear under mechanical loads for atoms in rows parallel to the axis of a screw dislocation and located near the nucleus of a dislocation and under dislocation slip conditions atoms can be accelerated up to energies much higher than the binding energy of atoms in a crystal. Fiz. Tverd. Tela (St. Petersburg) 39, 499–504 (March 1997)     

Formation and diffusion of self-interstitial atoms in silicon crystals under hydrostatic pressure: Quantum-chemical simulation

A theoretical modeling of the formation of Frenkel pairs and the diffusion of a self-interstitial atom in silicon crystals at normal and high (hydrostatic) pressures has been performed using molecular dynamics, semiempirical quantum-chemical (NDDO-PM5, PM6), and ab initio (SIESTA) methods. It is shown that, in a silicon crystal, the most stable configuration of a self-interstitial atom in the neutral charge state (I ⁰) is the split configuration 〈110〉. The shifted tetrahedral configuration (T ₁) is stable in the singlet and triplet excited states, as well as in the charge state Z = +2. The split 〈110〉 interstitial configuration remains stable under hydrostatic pressure (P ≤ 80 kbar). The activation barriers for diffusion of self-interstitial atoms in silicon crystals are determined to be as follows: ΔE _a (Si)(〈110〉 → T ₁) = 0.59 eV, ΔE _a (Si)(T ₁ → T′₁) = 0.1 eV, and ΔE _a (Si)(T ₁ → 〈110〉) = 0.23 eV. The hydrostatic pressure (P ≤ 80 kbar) increases the activation barrier for diffusion of self-interstitial atoms in silicon crystals. The energies of the formation of a separate Frenkel pair, a self-interstitial atom, and a vacancy are determined. It is demonstrated that the hydrostatic pressure decreases the energy of the formation of Frenkel pairs.     

Elastic properties of nanocrystalline forsterite under high pressure and high temperature

A simple theoretical model is developed to study the pressure–volume–temperature relationship and applied for nanocrystalline forsterite in the temperature range 300–1573 K and pressure range 0–9.6 GPa. The results obtained with the present model are in quite close agreement to the experimental values. The model is therefore extended to study the variation of bulk modulus and the coefficient of volume thermal expansion under high pressure and high temperature. The present study also reveals that the quasi-harmonic approximation, i.e., the product of bulk modulus and the coefficient of volume thermal expansion as constant, is valid at least up to the temperature 1573 K and pressure 9.6 GPa in case of nanocrystalline forsterite.     

Nonadiabatic effects in the lattice dynamics of compressed rare-gas crystals

Electron-ion contributions to the energy of rare-gas crystals are discussed from first principles in the framework of the Tolpygo model and its variants. The frequencies of phonons in a neon crystal at pressures p ≠ 0 are calculated in terms of models that go beyond the scope of the adiabatic approximation. Analysis of the contributions from different interactions to the lattice dynamics of the crystals demonstrates that the phonon frequencies calculated in the framework of the simplest model (allowing only for the nearest neighbors) and the most complex model (with the inclusion of the nearest neighbors, next-nearest neighbors, nonadiabatic effects, etc.) for small wave vectors are close to each other. The difference between the phonon frequencies calculated within the above models is most pronounced at the Brillouin zone boundary. Under strong compression, the phonon spectrum along the Δ direction is distorted and the longitudinal mode is softened as a result of the electron-phonon interaction. The contribution from terms of higher orders in the overlap integral S at p ≠ 0 to the phonon frequencies is more significant than that obtained in the band-structure calculations of the neon crystal.     

Overall values of conventional discrepancy indices for crystals with heavy atoms. Part I—Results for a triclinic crystal when the model consists of the heavy atoms and a part of light atoms

The joint probability density functions of the normalized structure amplitudes of the structure and the model (i.e.,y _N andy _p ^c ) are derived for triclinic crystals containing heavy atoms (1, 2 and many) by taking the model to consist of the heavy atoms and a part of the light atoms in the unit cell. These functions are derived for the two cases where the model is completely correct (i.e., the related case) and where the model is completely wrong (i.e., the unrelated case) in terms of the fractional contributions to the local mean intensity from the heavy atoms and all known atoms (i.e., σ _1h ^/2 and σ ₁ ² ) as parameters. These functions are then used to obtain the theoretical local values of 〈y _N〉 and 〈|y _N ⁿ − σ ₁ ⁿ (y _P ^c ) ⁿ |〉,n=1, 2. A method of using these results to compute the theoretical overall values ofR(F) andR(I) for the related and unrelated cases is briefly described. A comparison of the observed values of these indices with their theoretical values for the related and unrelated cases would help in determining the correctness of the proposed trial structure. Contribution No. 548     

Scattering of Stark-decelerated OH radicals with rare-gas atoms

We present a combined experimental and theoretical study on the rotationally inelastic scattering of OH (X²Π_3/2, J = 3/2, f) radicals with the collision partners He, Ne, Ar, Kr, Xe, and D₂ as a function of the collision energy between ～70 cm^?1 and 400 cm^?1. The OH radicals are state selected and velocity tuned prior to the collision using a Stark decelerator, and field-free parity-resolved state-to-state inelastic relative scattering cross sections are measured in a crossed molecular beam configuration. For all OH-rare gas atom systems excellent agreement is obtained with the cross sections predicted by coupled channel scattering calculations based on accurate ab initio potential energy surfaces. This series of experiments complements recent studies on the scattering of OH radicals with Xe [J.J. Gilijamse, S. Hoekstra, S.Y.T. van de Meerakker, G.C. Groenenboom, G. Meijer, Science 313, 1617 (2006)], Ar [L. Scharfenberg, J. K?os, P.J. Dagdigian, M.H. Alexander, G. Meijer, S.Y.T. van de Meerakker, Phys. Chem. Chem. Phys. 12, 10660 (2010)], He, and D₂ [M. Kirste, L. Scharfenberg, J. K?os, F. Lique, M.H. Alexander, G. Meijer, S.Y.T. van de Meerakker, Phys. Rev. A 82, 042717 (2010)]. A comparison of the relative scattering cross sections for this set of collision partners reveals interesting trends in the scattering behavior.     

Elastic properties of metastable crystalline and amorphous gasb-ge semiconductors synthesized under high pressure

We present the systematic study of the elastic shear G and bulk B moduli in amorphous and crystalline metastable ternary solid solutions (GaSb)_1?x Ge_2x . It is found that the moduli of crystalline phases initially decrease with Ge concentration, falling down to minimum values at 20-30% Ge. The minimal values of elastic moduli for amorphous samples are observed at 50-60% Ge. Elastic softness of crystalline solid solutions is assumed to be related to the increase of chemical disorder and, consequently, of static (non-thermal) geometrical disorder in positions of atoms. An additional topological disorder in amorphous solid solutions leads to additional elastic softening.