58 research outputs found
Data-driven simulation and characterisation of gold nanoparticle melting
The simulation and analysis of the thermal stability of nanoparticles, a stepping stone towards their application in technological devices, require fast and accurate force fields, in conjunction with effective characterisation methods. In this work, we develop efficient, transferable, and interpretable machine learning force fields for gold nanoparticles based on data gathered from Density Functional Theory calculations. We use them to investigate the thermodynamic stability of gold nanoparticles of different sizes (1 to 6 nm), containing up to 6266 atoms, concerning a solid-liquid phase change through molecular dynamics simulations. We predict nanoparticle melting temperatures in good agreement with available experimental data. Furthermore, we characterize the solid-liquid phase change mechanism employing an unsupervised learning scheme to categorize local atomic environments. We thus provide a data-driven definition of liquid atomic arrangements in the inner and surface regions of a nanoparticle and employ it to show that melting initiates at the outer layers
Surface Phase Transitions Induced by Electron Mediated Adatom-Adatom Interaction
We propose that the indirect adatom-adatom interaction mediated by the
conduction electrons of a metallic surface is responsible for the
structural phase transitions
observed in Sn/Ge (111) and Pb/Ge (111). When the indirect interaction
overwhelms the local stress field imposed by the substrate registry, the system
suffers a phonon instability, resulting in a structural phase transition in the
adlayer. Our theory is capable of explaining all the salient features of the
transitions observed in
Sn/Ge (111) and Pb/Ge (111), and is in principle applicable to a wide class of
systems whose surfaces are metallic before the transition.Comment: 4 pages, 5 figure
Templated growth of metal-organic coordination chains at surfaces
Line them up: Metal\u2013organic chains (see scanning tunneling microscopy image) have been created in situ by self\u2010organized growth at a metal surface under ultrahigh vacuum. These 1D arrangements of metal centers (Fe, Cu), regularly spaced by organic linkers such as trimesitylic acid, open new possibilities for the study of low\u2010dimensional magnetism
Enhancement of piezoelectricity in a mixed ferroelectric
We use first-principles density-functional total energy and polarization
calculations to calculate the piezoelectric tensor at zero temperature for both
cubic and simple tetragonal ordered supercells of Pb_3GeTe_4. The largest
piezoelectric coefficient for the tetragonal configuration is enhanced by a
factor of about three with respect to that of the cubic configuration. This can
be attributed to both the larger strain-induced motion of cations relative to
anions and higher Born effective charges in the tetragonal case. A normal mode
decomposition shows that both cation ordering and local relaxation weaken the
ferroelectric instability, enhancing piezoelectricity.Comment: 5 pages, revtex, 2 eps figure
Magnons in real materials from density-functional theory
We present an implementation of the adiabatic spin-wave dynamics of Niu and
Kleinman. This technique allows to decouple the spin and charge excitations of
a many-electron system using a generalization of the adiabatic approximation.
The only input for the spin-wave equations of motion are the energies and Berry
curvatures of many-electron states describing frozen spin spirals. The latter
are computed using a newly developed technique based on constrained
density-functional theory, within the local spin density approximation and the
pseudo-potential plane-wave method. Calculations for iron show an excellent
agreement with experiments.Comment: 1 LaTeX file and 1 postscript figur
Determination of the (3x3)-Sn/Ge(111) structure by photoelectron diffraction
At a coverage of about 1/3 monolayer, Sn deposited on Ge(111) below 550 forms
a metastable (sqrt3 x sqrt3)R30 phase. This phase continuously and reversibly
transforms into a (3x3) one, upon cooling below 200 K. The photoemission
spectra of the Sn 4d electrons from the (3x3)-Sn/Ge(111) surface present two
components which are attributed to inequivalent Sn atoms in T4 bonding sites.
This structure has been explored by photoelectron diffraction experiments
performed at the ALOISA beamline of the Elettra storage ring in Trieste
(Italy). The modulation of the intensities of the two Sn components, caused by
the backscattering of the underneath Ge atoms, has been measured as a function
of the emission angle at fixed kinetic energies and viceversa. The bond angle
between Sn and its nearest neighbour atoms in the first Ge layer (Sn-Ge1) has
been measured by taking polar scans along the main symmetry directions and it
was found almost equivalent for the two components. The corresponding bond
lengths are also quite similar, as obtained by studying the dependence on the
photoelectron kinetic energy, while keeping the photon polarization and the
collection direction parallel to the Sn-Ge1 bond orientation (bond emission). A
clear difference between the two bonding sites is observed when studying the
energy dependence at normal emission, where the sensitivity to the Sn height
above the Ge atom in the second layer is enhanced. This vertical distance is
found to be 0.3 Angstroms larger for one Sn atom out of the three contained in
the lattice unit cell. The (3x3)-Sn/Ge(111) is thus characterized by a
structure where the Sn atom and its three nearest neighbour Ge atoms form a
rather rigid unit that presents a strong vertical distortion with respect to
the underneath atom of the second Ge layer.Comment: 10 pages with 9 figures, added reference
Role of defects in the electronic properties of amorphous/crystalline Si interface
The mechanism determining the band alignment of the amorphous/crystalline
Si heterostructures is addressed with direct atomistic simulations of the
interface performed using a hierarchical combination of various computational
schemes ranging from classical model-potential molecular dynamics to ab-initio
methods. We found that in coordination defect-free samples the band alignment
is almost vanishing and independent on interface details. In defect-rich
samples, instead, the band alignment is sizeably different with respect to the
defect-free case, but, remarkably, almost independent on the concentration of
defects. We rationalize these findings within the theory of semiconductor
interfaces.Comment: 4 pages in two-column format, 2 postscript figures include
Virtual-crystal approximation that works: Locating a composition phase boundary in Pb(Zr_{1-x}Ti_3)O_3
We present a new method for modeling disordered solid solutions, based on the
virtual crystal approximation (VCA). The VCA is a tractable way of studying
configurationally disordered systems; traditionally, the potentials which
represent atoms of two or more elements are averaged into a composite atomic
potential. We have overcome significant shortcomings of the standard VCA by
developing a potential which yields averaged atomic properties. We perform the
VCA on a ferroelectric oxide, determining the energy differences between the
high-temperature rhombohedral, low-temperature rhombohedral and tetragonal
phases of Pb(Zr_{1-x}Ti_x)O_3 at x=0.5 and comparing these results to
superlattice calculations and experiment. We then use our new method to
determine the preferred structural phase at x=0.4. We find that the
low-temperature rhombohedral phase becomes the ground state at x=0.4, in
agreement with experimental findings.Comment: 5 pages, no figure
Phonons and related properties of extended systems from density-functional perturbation theory
This article reviews the current status of lattice-dynamical calculations in
crystals, using density-functional perturbation theory, with emphasis on the
plane-wave pseudo-potential method. Several specialized topics are treated,
including the implementation for metals, the calculation of the response to
macroscopic electric fields and their relevance to long wave-length vibrations
in polar materials, the response to strain deformations, and higher-order
responses. The success of this methodology is demonstrated with a number of
applications existing in the literature.Comment: 52 pages, 14 figures, submitted to Review of Modern Physic
Photoelasticity of crystalline and amorphous silica from first principles
Based on density-functional perturbation theory we have computed from first
principles the photoelastic tensor of few crystalline phases of silica at
normal conditions and high pressure (quartz, -cristobalite,
-cristobalite) and of models of amorphous silica (containig up to 162
atoms), obtained by quenching from the melt in combined classical and
Car-Parrinello molecular dynamics simulations. The computational framework has
also been checked on the photoelastic tensor of crystalline silicon and MgO as
prototypes of covalent and ionic systems. The agreement with available
experimental data is good.
A phenomenological model suitable to describe the photoelastic properties of
different silica polymorphs is devised by fitting on the ab-initio data.Comment: ten figure
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