Towards a first principles description of phonons in Ni50_{50}Pt50_{50} disordered alloys: the role of relaxation

Using a combination of density-functional perturbation theory and the itinerant coherent potential approximation, we study the effects of atomic relaxation on the inelastic incoherent neutron scattering cross sections of disordered Ni$_{50}$Pt$_{50}$ alloys. We build on previous work, where empirical force constants were adjusted {\it ad hoc} to agree with experiment. After first relaxing all structural parameters within the local-density approximation for ordered NiPt compounds, density-functional perturbation theory is then used to compute phonon spectra, densities of states, and the force constants. The resulting nearest-neighbor force constants are first compared to those of other ordered structures of different stoichiometry, and then used to generate the inelastic scattering cross sections within the itinerant coherent potential approximation. We find that structural relaxation substantially affects the computed force constants and resulting inelastic cross sections, and that the effect is much more pronounced in random alloys than in ordered alloys.Comment: 8 pages, 3 eps figures, uses revtex

Inelastic neutron scattering in random binary alloys : an augmented space approach

Combining the augmented space representation for phonons with a generalized version of Yonezawa-Matsubara diagrammatic technique, we have set up a formalism to seperate the coherent and incoherent part of the total intensity of thermal neutron scattering from disordered alloys. This is done exacly without taking any recourse to mean-field like approximation (as done previously). The formalism includes disorder in masses, force constants and scattering lengths. Implementation of the formalism to realistic situations is performed by an augmented space Block recursion which calculates entire Green matrix and self energy matrix which in turn is needed to evaluate the coherent and incoherent intensities. we apply the formalism to NiPd and NiPt alloys. Numerical results on coherent and incoherent scattering cross sections are presented along the highest symmetry directions. Finally the incoherent intensities are compared with the CPA and also with experiments.Comment: 18 pages, 13 figure

Phonon densities of states and vibrational entropies of ordered and disordered Ni3Al

We performed inelastic neutron-scattering measurements on powdered Ni3Al. The alloy was prepared in two states of chemical order: (1) with equilibrium L12 order, and (2) with disorder (the material was a fcc solid solution prepared by high-energy ball milling). Procedures to convert the energy loss spectra into approximate phonon density of states (DOS) curves for Ni3Al in the two states of chemical order were guided by Born–von Kármán analyses with force constants obtained from previous single-crystal experiments on L12-ordered Ni3Al and fcc Ni metal. The main difference in the phonon DOS of the ordered and disordered alloys occurs near 39 meV, the energy of a peak arising from optical modes in the ordered alloy. These high-frequency optical modes involve primarily the vibrations of the aluminum-rich sublattice. The disordered alloy, which does not have such a sublattice, shows much less intensity at this energy. This difference in the phonon DOS around 39 meV is the main contributor to the difference in vibrational entropy of disordered and ordered Ni3Al, which we estimate to be Svibdis-Svibord=(+0.2±0.1)kB/atom at high temperatures

Structure and Vibrations of the Vicinal Copper (211) Surface

We report a first principles theoretical study of the surface relaxation and lattice dynamics of the Cu(211) surface using the plane wave pseudopotential method. We find large atomic relaxations for the first several atomic layers near the step edges on this surface, and a substantial step-induced renormalization of the surface harmonic force constants. We use the results to study the harmonic fluctuations around the equilibrium structure and find three new step-derived features in the zone center vibrational spectrum. Comparison of these results with previous theoretical work and weith experimental studies using inelastic He scattering are reported.Comment: 6 Pages RevTex, 7 Figures in Postscrip

Anisotropic Condensation of Helium in Nanotube Bundles

Helium atoms are strongly attracted to the interstitial channels within a bundle of carbon nanotubes. The strong corrugation of the axial potential within a channel can produce a lattice gas system where the weak mutual attraction between atoms in neighboring channels of a bundle induces condensation into a remarkably anisotropic phase with very low binding energy. We estimate the binding energy and critical temperature for 4He in this novel quasi-one-dimensional condensed state. At low temperatures, the specific heat of the adsorbate phase (fewer than 2% of the total number of atoms) greatly exceeds that of the host material.Comment: 8 pages, 3 figures, submitted to PRL (corrected typo in abstract

H2 in the interstitial channels of nanotube bundles

The equation of state of H2 adsorbed in the interstitial channels of a carbon nanotube bundle has been calculated using the diffusion Monte Carlo method. The possibility of a lattice dilation, induced by H2 adsorption, has been analyzed by modeling the cohesion energy of the bundle. The influence of factors like the interatomic potentials, the nanotube radius and the geometry of the channel on the bundle swelling is systematically analyzed. The most critical input is proved to be the C-H2 potential. Using the same model than in planar graphite, which is expected to be also accurate in nanotubes, the dilation is observed to be smaller than in previous estimations or even inexistent. H2 is highly unidimensional near the equilibrium density, the radial degree of freedom appearing progressively at higher densities.Comment: Accepted for publication in PR

Determination of the Bending Rigidity of Graphene via Electrostatic Actuation of Buckled Membranes

The small mass and atomic-scale thickness of graphene membranes make them highly suitable for nanoelectromechanical devices such as e.g. mass sensors, high frequency resonators or memory elements. Although only atomically thick, many of the mechanical properties of graphene membranes can be described by classical continuum mechanics. An important parameter for predicting the performance and linearity of graphene nanoelectromechanical devices as well as for describing ripple formation and other properties such as electron scattering mechanisms, is the bending rigidity, {\kappa}. In spite of the importance of this parameter it has so far only been estimated indirectly for monolayer graphene from the phonon spectrum of graphite, estimated from AFM measurements or predicted from ab initio calculations or bond-order potential models. Here, we employ a new approach to the experimental determination of {\kappa} by exploiting the snap-through instability in pre-buckled graphene membranes. We demonstrate the reproducible fabrication of convex buckled graphene membranes by controlling the thermal stress during the fabrication procedure and show the abrupt switching from convex to concave geometry that occurs when electrostatic pressure is applied via an underlying gate electrode. The bending rigidity of bilayer graphene membranes under ambient conditions was determined to be $35.5^{+20}_{-15}$ eV. Monolayers have significantly lower {\kappa} than bilayers

Phonon and plasmon excitation in inelastic electron tunneling spectroscopy of graphite

The inelastic electron tunneling spectrum (IETS)of highly oriented pyrolitic graphite (HOPG) has been measured with scanning tunneling spectroscopy (STS) at 6K. The observed spectral features are in very good agreement with the vibrational density of states (vDOS) of graphite calculated from first principles. We discuss the enhancement of certain phonon modes by phonon-assisted tunneling in STS based on the restrictions imposed by the electronic structure of graphite. We also demonstrate for the first time the local excitation of surface-plasmons in IETS which are detected at an energy of 40 meV.Comment: PRB rapid communication, submitte

Vibrations of a chain of Xe atoms in a groove of carbon nanotube bundle

We present a lattice dynamics study of the vibrations of a linear chain of Xe adsorbates in groove positions of a bundle of carbon nanotubes. The characteristic phonon frequencies are calculated and the adsorbate polarization vectors discussed. Comparison of the present results with the ones previously published shows that the adsorbate vibrations cannot be treated as completely decoupled from the vibrations of carbon nanotubes and that a significant hybridization between the adsorbate and the tube modes occurs for phonons of large wavelengths.Comment: 3 PS figure

Coil Formation in Multishell Carbon Nanotubes: Competition between Curvature Elasticity and Interlayer Adhesion

To study the shape formation process of carbon nanotubes, a string equation describing the possible existing shapes of the axis-curve of multishell carbon tubes (MCTs) is obtained in the continuum limit by minimizing the shape energy, that is the difference between the MCT energy and the energy of the carbonaceous mesophase (CM). It is shown that there exists a threshold relation of the outmost and inmost radii, that gives a parameter regime in which a straight MCT will be bent or twisted. Among the deformed shapes, the regular coiled MCTs are shown being one of the solutions of the string equation. In particular,the optimal ratio of pitch $p$ and radius $r_0$ for such a coil is found to be equal to $2\pi$, which is in good agreement with recent observation of coil formation in MCTs by Zhang et al.Comment: RevTeX, no figure, 12 pages, to appear in Phys. Rev. Let