Search results for "Statistical"
showing 10 items of 4960 documents
On fermionic shadow wave functions for strongly correlated multi-reference systems based on a single Slater determinant
2015
We demonstrate that extending the Shadow Wave Function to fermionic systems facilitates to accurately calculate strongly-correlated multi-reference systems such as the stretched H2 molecule. This development considerably extends the scope of electronic structure calculations and enables to efficiently recover the static correlation energy using just a single Slater determinant.
Nuclear quantum effects in liquid water from path-integral simulations using anab initioforce-matching approach
2014
We have applied path integral simulations, in combination with new ab initio based water potentials, to investigate nuclear quantum effects in liquid water. Because direct ab initio path integral simulations are computationally expensive, a flexible water model is parameterized by force-matching to density functional theory-based molecular dynamics simulations. The resulting effective potentials provide an inexpensive replacement for direct ab inito molecular dynamics simulations and allow efficient simulation of nuclear quantum effects. Static and dynamic properties of liquid water at ambient conditions are presented and the role of nuclear quantum effects, exchange-correlation functionals…
The adiabatic strictly-correlated-electrons functional : kernel and exact properties
2016
We investigate a number of formal properties of the adiabatic strictly-correlated electrons (SCE) functional, relevant for time-dependent potentials and for kernels in linear response time-dependent density functional theory. Among the former, we focus on the compliance to constraints of exact many-body theories, such as the generalised translational invariance and the zero-force theorem. Within the latter, we derive an analytical expression for the adiabatic SCE Hartree exchange-correlation kernel in one dimensional systems, and we compute it numerically for a variety of model densities. We analyse the non-local features of this kernel, particularly the ones that are relevant in tackling p…
Dynamic Self-Consistent Field Approach for Studying Kinetic Processes in Multiblock Copolymer Melts
2020
The self-consistent field theory is a popular and highly successful theoretical framework for studying equilibrium (co)polymer systems at the mesoscopic level. Dynamic density functionals allow one to use this framework for studying dynamical processes in the diffusive, non-inertial regime. The central quantity in these approaches is the mobility function, which describes the effect of chain connectivity on the nonlocal response of monomers to thermodynamic driving fields. In a recent study [Mantha et al, Macromolecules 53, 3409 (2020)], we have developed a method to systematically construct mobility functions from reference fine-grained simulations. Here we focus on melts of linear chains …
Cavity-induced bifurcation in classical rate theory
2022
We show how coupling an ensemble of bistable systems to a common cavity field affects the collective stochastic behavior of this ensemble. In particular, the cavity provides an effective interaction between the systems, and parametrically modifies the transition rates between the metastable states. We predict that the cavity induces a collective phase transition at a critical temperature which depends linearly on the number of systems. It shows up as a spontaneous symmetry breaking where the stationary states of the bistable system bifurcate. We observe that the transition rates slow down independently of the phase transition, but the rate modification vanishes for alternating signs of the …
Recent achievements in ab initio modelling of liquid water
2013
The application of newly developed first-principle modeling techniques to liquid water deepens our understanding of the microscopic origins of its unusual macroscopic properties and behaviour. Here, we review two novel ab initio computational methods: second-generation Car-Parrinello molecular dynamics and decomposition analysis based on absolutely localized molecular orbitals. We show that these two methods in combination not only enable ab initio molecular dynamics simulations on previously inaccessible time and length scales, but also provide unprecedented insights into the nature of hydrogen bonding between water molecules. We discuss recent applications of these methods to water cluste…
Levy flights in confining environments: Random paths and their statistics
2013
We analyze a specific class of random systems that are driven by a symmetric L\'{e}vy stable noise. In view of the L\'{e}vy noise sensitivity to the confining "potential landscape" where jumps take place (in other words, to environmental inhomogeneities), the pertinent random motion asymptotically sets down at the Boltzmann-type equilibrium, represented by a probability density function (pdf) $\rho_*(x) \sim \exp [-\Phi (x)]$. Since there is no Langevin representation of the dynamics in question, our main goal here is to establish the appropriate path-wise description of the underlying jump-type process and next infer the $\rho (x,t)$ dynamics directly from the random paths statistics. A pr…
Modeling of biomolecular machines in non-equilibrium steady states
2021
Numerical computations have become a pillar of all modern quantitative sciences. Any computation involves modeling--even if often this step is not made explicit--and any model has to neglect details while still being physically accurate. Equilibrium statistical mechanics guides both the development of models and numerical methods for dynamics obeying detailed balance. For systems driven away from thermal equilibrium such a universal theoretical framework is missing. For a restricted class of driven systems governed by Markov dynamics and local detailed balance, stochastic thermodynamics has evolved to fill this gap and to provide fundamental constraints and guiding principles. The next step…
Microstructure–property relation and machine learning prediction of hole expansion capacity of high-strength steels
2021
Abstract The relationship between microstructure features and mechanical properties plays an important role in the design of materials and improvement of properties. Hole expansion capacity plays a fundamental role in defining the formability of metal sheets. Due to the complexity of the experimental procedure of testing hole expansion capacity, where many influencing factors contribute to the resulting values, the relationship between microstructure features and hole expansion capacity and the complexity of this relation is not yet fully understood. In the present study, an experimental dataset containing the phase constituents of 55 microstructures as well as corresponding properties, su…
Archaeometry of Sicilian glazed pottery
2004
Petrographic and chemical analyses of the “ceramic body” of 114 majolica artefacts manufactured in Sicily over a wide time range (16th–-19th century) are presented. All the analysed samples, which belong to museums and private collections, were previously attributed to Sicilian workshops based on stylistic features evaluated by expert historians of art. Unambiguous identification of the production sites of majolica handicrafts in Sicily remains, however, open to question when this relies only on purely stylistic considerations. To this end compositional and/or textural markers have been searched for in the “ceramic body” of the majolica artefacts in order to differentiate between the centre…