22,463 research outputs found
Scanning tunneling microscopy simulations of poly(3-dodecylthiophene) chains adsorbed on highly oriented pyrolytic graphite
We report on a novel scheme to perform efficient simulations of Scanning
Tunneling Microscopy (STM) of molecules weakly bonded to surfaces. Calculations
are based on a tight binding (TB) technique including self-consistency for the
molecule to predict STM imaging and spectroscopy. To palliate the lack of
self-consistency in the tunneling current calculation, we performed first
principles density-functional calculations to extract the geometrical and
electronic properties of the system. In this way, we can include, in the TB
scheme, the effects of structural relaxation upon adsorption on the electronic
structure of the molecule. This approach is applied to the study of
regioregular poly(3-dodecylthiophene) (P3DDT) polymer chains adsorbed on highly
oriented pyrolytic graphite (HOPG). Results of spectroscopic calculations are
discussed and compared with recently obtained experimental datComment: 15 pages plus 5 figures in a tar fil
Band Gap Modulation of Graphene on SiC
A recipe on how to engineer a band gap in the energy spectrum for the
carriers in graphene is conveyed. It is supported by a series of numerical
simulations inspired by an analytical result based on the opening of a band gap
in periodically corrugated graphene, e.g. the buffer layer grown on SiC at high
temperatures.Comment: accepted in EPJ
Large scale ab-initio simulations of dislocations
We present a novel methodology to compute relaxed dislocations core configurations, and their energies in crystalline metallic materials using large-scale ab-intio simulations. The approach is based on MacroDFT, a coarse-grained density functional theory method that accurately computes the electronic structure with sub-linear scaling resulting in a tremendous reduction in cost. Due to its implementation in real-space, MacroDFT has the ability to harness petascale resources to study materials and alloys through accurate ab-initio calculations. Thus, the proposed methodology can be used to investigate dislocation cores and other defects where long range elastic effects play an important role, such as in dislocation cores, grain boundaries and near precipitates in crystalline materials. We demonstrate the method by computing the relaxed dislocation cores in prismatic dislocation loops and dislocation segments in magnesium (Mg). We also study the interaction energy with a line of Aluminum (Al) solutes. Our simulations elucidate the essential coupling between the quantum mechanical aspects of the dislocation core and the long range elastic fields that they generate. In particular, our quantum mechanical simulations are able to describe the logarithmic divergence of the energy in the far field as is known from classical elastic theory. In order to reach such scaling, the number of atoms in the simulation cell has to be exceedingly large, and cannot be achieved with the state-of-the-art density functional theory implementations
Direct Wolf summation of a polarizable force field for silica
We extend the Wolf direct, pairwise r^(-1) summation method with spherical
truncation to dipolar interactions in silica. The Tangney-Scandolo interatomic
force field for silica takes regard of polarizable oxygen atoms whose dipole
moments are determined by iteration to a self-consistent solution. With Wolf
summation, the computational effort scales linearly in the system size and can
easily be distributed among many processors, thus making large-scale
simulations of dipoles possible. The details of the implementation are
explained. The approach is validated by estimations of the error term and
simulations of microstructural and thermodynamic properties of silica.Comment: See http://link.aip.org/link/?JCP/132/194109 - 8 pages, 6 figures.
Changes in v3: Copyright notice added, minor typographical changes. Changes
in v2: 1. Inserted Paragraph in Sec. IV B describing the limitations of the
TS potential. 2. We corrected transcription errors in Tab. II, and adjusted
the deviation percentages mentioned in Sec. IV B, first paragraph,
accordingl
Extension of the QuickFF force field protocol for an improved accuracy of structural, vibrational, mechanical and thermal properties of metal-organic frameworks
QuickFF was originally launched in 2015 to derive accurate force fields for isolated and complex molecular systems in a quick and easy way. Apart from the general applicability, the functionality was especially tested for metal-organic frameworks (MOFs), a class of hybrid materials consisting of organic and inorganic building blocks. Herein, we launch a new release of the QuickFF protocol which includes new major features to predict structural, vibrational, mechanical and thermal properties with greater accuracy, without compromising its robustness and transparent workflow. First, the ab initio data necessary for the fitting procedure may now also be derived from periodic models for the molecular system, as opposed to the earlier cluster-based models. This is essential for an accurate description of MOFs with one-dimensional metal-oxide chains. Second, cross terms that couple internal coordinates (ICs) and anharmonic contributions for bond and bend terms are implemented. These features are essential for a proper description of vibrational and thermal properties. Third, the fitting scheme was modified to improve robustness and accuracy. The new features are tested on MIL-53(Al), MOF-5, CAU-13 and NOTT-300. As expected, periodic input data are proven to be essential for a correct description of structural, vibrational and thermodynamic properties of MIL-53(Al). Bulk moduli and thermal expansion coefficients of MOF-5 are very accurately reproduced by static and dynamic simulations using the newly derived force fields which include cross terms and anharmonic corrections. For the flexible materials CAU-13 and NOTT-300, the transition pressure is accurately predicted provided cross terms are taken into account
Spiral graphone and one sided fluorographene nano-ribbons
The instability of a free-standing one sided hydrogenated/fluorinated
graphene nano-ribbon, i.e. graphone/fluorographene, is studied using ab-initio,
semiempirical and large scale molecular dynamics simulations. Free standing
semi-infinite arm-chair like hydrogenated/fluorinated graphene (AC-GO/AC-GF)
and boat like hydrogenated/fluorinated graphene (B-GO/B-GF) (nano-ribbons which
are periodic along the zig-zag direction) are unstable and spontaneously
transform into spiral structures. We find that rolled, spiral B-GO and B-GF are
energetically more favorable than spiral AC-GO and AC-GF which is opposite to
the double sided flat hydrogenated/fluorinated graphene, i.e.
graphane/fluorographene. We found that the packed, spiral structures exhibit
unexpected localized HOMO-LUMO at the edges with increasing energy gap during
rolling. These rolled hydrocarbon structures are stable beyond room temperature
up to at least =1000\,K.Comment: Phys. Rev. B 87, 075448 (2013
Ab initio atomistic thermodynamics and statistical mechanics of surface properties and functions
Previous and present "academic" research aiming at atomic scale understanding
is mainly concerned with the study of individual molecular processes possibly
underlying materials science applications. Appealing properties of an
individual process are then frequently discussed in terms of their direct
importance for the envisioned material function, or reciprocally, the function
of materials is somehow believed to be understandable by essentially one
prominent elementary process only. What is often overlooked in this approach is
that in macroscopic systems of technological relevance typically a large number
of distinct atomic scale processes take place. Which of them are decisive for
observable system properties and functions is then not only determined by the
detailed individual properties of each process alone, but in many, if not most
cases also the interplay of all processes, i.e. how they act together, plays a
crucial role. For a "predictive materials science modeling with microscopic
understanding", a description that treats the statistical interplay of a large
number of microscopically well-described elementary processes must therefore be
applied. Modern electronic structure theory methods such as DFT have become a
standard tool for the accurate description of individual molecular processes.
Here, we discuss the present status of emerging methodologies which attempt to
achieve a (hopefully seamless) match of DFT with concepts from statistical
mechanics or thermodynamics, in order to also address the interplay of the
various molecular processes. The new quality of, and the novel insights that
can be gained by, such techniques is illustrated by how they allow the
description of crystal surfaces in contact with realistic gas-phase
environments.Comment: 24 pages including 17 figures, related publications can be found at
http://www.fhi-berlin.mpg.de/th/paper.htm
Computing energy barriers for rare events from hybrid quantum/classical simulations through the virtual work principle
Hybrid quantum/classical techniques can flexibly couple ab initio simulations
to an empirical or elastic medium to model materials systems that cannot be
contained in small periodic supercells. However, due to electronic non-locality
a total energy cannot be defined, meaning energy barriers cannot be calculated.
We provide a general solution using the principle of virtual work in a modified
nudged elastic band algorithm. Our method enables the first ab initio
calculations of the kink formation energy for edge dislocations in
molybdenum and lattice trapping barriers to brittle fracture in silicon
- …