6,916 research outputs found
Low-temperature anharmonicity of barium titanate: a path-integral molecular dynamics study
We investigate the influence of quantum effects on the dielectric and
piezoelectric properties of barium titanate in its (low-temperature)
rhombohedral phase, and show the strongly anharmonic character of this system
even at low temperature. For this purpose, we perform path-integral
molecular-dynamics simulations under fixed pressure and fixed temperature,
using an efficient Langevin thermostat-barostat, and an effective hamiltonian
derived from first-principles calculations. The quantum fluctuations are shown
to significantly enhance the static dielectric susceptibility (~ by a factor 2)
and the piezoelectric constants, reflecting the strong anharmonicity of this
ferroelectric system even at very low temperature. The slow
temperature-evolution of the dielectric properties observed below ~ 100 K is
attributed (i) to zero-point energy contributions and (ii) to harmonic behavior
if quantum effects are turned off.Comment: submitted to Phys. Rev.
Mass Density Fluctuations in Quantum and Classical descriptions of Liquid Water
First principles molecular dynamics simulation protocol is established using
revised functional of Perdew-Burke-Ernzerhof (revPBE) in conjunction with
Grimme's third generation of dispersion (D3) correction to describe properties
of water at ambient conditions. This study also demonstrates the consistency of
the structure of water across both isobaric (NpT) and isothermal (NVT)
ensembles. Going beyond the standard structural benchmarks for liquid water, we
compute properties that are connected to both local structure and mass density
uctuations that are related to concepts of solvation and hydrophobicity. We
directly compare our revPBE results to the Becke-Lee-Yang-Parr (BLYP) plus
Grimme dispersion corrections (D2) and both the empirical fixed charged model
(SPC/E) and many body interaction potential model (MB-pol) to further our
understanding of how the computed properties herein depend on the form of the
interaction potential
Shear stress relaxation and ensemble transformation of shear stress autocorrelation functions revisited
We revisit the relation between the shear stress relaxation modulus ,
computed at finite shear strain , and the shear stress
autocorrelation functions and computed,
respectively, at imposed strain and mean stress . Focusing on
permanent isotropic spring networks it is shown theoretically and
computationally that in general
for with being the static equilibrium shear modulus.
and thus must become different for solids and it is impossible
to obtain alone from as often assumed. We comment
briefly on self-assembled transient networks where must vanish for
a finite scission-recombination frequency . We argue that should reveal an intermediate plateau set by the
shear modulus of the quenched network.Comment: 8 pages, 4 figure
Aging and Energy Landscapes: Application to Liquids and Glasses
The equation of state for a liquid in equilibrium, written in the potential
energy landscape formalism, is generalized to describe out-of-equilibrium
conditions. The hypothesis that during aging the system explores basins
associated to equilibrium configurations is the key ingredient in the
derivation. Theoretical predictions are successfully compared with data from
molecular dynamics simulations of different aging processes, such as
temperature and pressure jumps.Comment: RevTeX4, 4 pages, 5 eps figure
Efficient potential of mean force calculation from multiscale simulations: solute insertion in a lipid membrane
The determination of potentials of mean force for solute insertion in a
membrane by means of all-atom molecular dynamics simulations is often hampered
by sampling issues. A multiscale approach to conformational sampling was
recently proposed by Bereau and Kremer (2016). It aims at accelerating the
sampling of the atomistic conformational space by means of a systematic
backmapping of coarse-grained snapshots. In this work, we first analyze the
efficiency of this method by comparing its predictions for propanol insertion
into a 1,2-Dimyristoyl-sn-glycero-3-phosphocholine membrane (DMPC) against
reference atomistic simulations. The method is found to provide accurate
results with a gain of one order of magnitude in computational time. We then
investigate the role of the coarse-grained representation in affecting the
reliability of the method in the case of a
1,2-Dioleoyl-sn-glycero-3-phosphocholine membrane (DOPC). We find that the
accuracy of the results is tightly connected to the presence a good
configurational overlap between the coarse-grained and atomistic models---a
general requirement when developing multiscale simulation methods.Comment: 6 pages, 5 figure
Challenges in first-principles NPT molecular dynamics of soft porous crystals: A case study on MIL-53(Ga)
Soft porous crystals present a challenge to molecular dynamics simulations
with flexible size and shape of the simulation cell (i.e., in the NPT
ensemble), since their framework responds very sensitively to small external
stimuli. Hence, all interactions have to be described very accurately in order
to obtain correct equilibrium structures. Here, we report a methodological
study on the nanoporous metal-organic framework MIL-53(Ga), which undergoes a
large-amplitude transition between a narrow- and a large-pore phase upon a
change in temperature. Since this system has not been investigated by density
functional theory (DFT)-based NPT simulations so far, we carefully check the
convergence of the stress tensor with respect to computational parameters.
Furthermore, we demonstrate the importance of dispersion interactions and test
two different ways of incorporating them into the DFT framework. As a result,
we propose two computational schemes which describe accurately the narrow- and
the large-pore phase of the material, respectively. These schemes can be used
in future work on the delicate interplay between adsorption in the nanopores
and structural flexibility of the host material
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