Search results for "physics.chem-ph"
showing 10 items of 359 documents
Efficient and portable acceleration of quantum chemical many-body methods in mixed floating point precision using OpenACC compiler directives
2016
It is demonstrated how the non-proprietary OpenACC standard of compiler directives may be used to compactly and efficiently accelerate the rate-determining steps of two of the most routinely applied many-body methods of electronic structure theory, namely the second-order M{\o}ller-Plesset (MP2) model in its resolution-of-the-identity (RI) approximated form and the (T) triples correction to the coupled cluster singles and doubles model (CCSD(T)). By means of compute directives as well as the use of optimized device math libraries, the operations involved in the energy kernels have been ported to graphics processing unit (GPU) accelerators, and the associated data transfers correspondingly o…
Quantum dynamics by the constrained adiabatic trajectory method
2011
We develop the constrained adiabatic trajectory method (CATM) which allows one to solve the time-dependent Schr\"odinger equation constraining the dynamics to a single Floquet eigenstate, as if it were adiabatic. This constrained Floquet state (CFS) is determined from the Hamiltonian modified by an artificial time-dependent absorbing potential whose forms are derived according to the initial conditions. The main advantage of this technique for practical implementation is that the CFS is easy to determine even for large systems since its corresponding eigenvalue is well isolated from the others through its imaginary part. The properties and limitations of the CATM are explored through simple…
Scientific and technological approaches for sintering and joining of metallic materials by SPS
2013
The flash sintering technique (commonly known as spark plasma sintering, SPS) generates a craze worldwide. This process allows a powder densification from speeds generally 10 to 100 times higher than those of the traditional sintering techniques. In addition, this allows the synthesis of innovative and original dense materials, with a controlled microstructure, complex shapes and, sometimes large sizes. However, the control of scaling and microstructure homogeneity of parts obtained by such a process requires a perfect knowledge of technical equipment including flash sintering to reduce thermal gradients. Modeling is a valuable aid to achieve the improvement of its control. Another potentia…
Bending Carbon Nanoforms for Supramolecular Recognition: A Topological Study on Hemifullerene-Based Aggregates
2018
International audience; Buckybowls have risen as appealing fullerene fragment derivatives. Their intrinsic curvature has been exploited in the generation of host–guest supramolecular assemblies, not only through concave–convex complementarity but also through less-known concave–concave staggered arrangements. Whereas the stabilization of bowl-in-bowl dispositions has been ascribed to efficient π–π forces together with favorable dipole–dipole interactions, a detailed analysis on the forces guiding the formation of the staggered arrangements is missing so far. Herein, we present a thorough theoretical characterization of bowl-in-bowl vs staggered hemifullerene-based homodimers and heterodimer…
Efficient and accurate modeling of electron photoemission in nanostructures with TDDFT
2017
We derive and extend the time-dependent surface-flux method introduced in [L. Tao, A. Scrinzi, New J. Phys. 14, 013021 (2012)] within a time-dependent density-functional theory (TDDFT) formalism and use it to calculate photoelectron spectra and angular distributions of atoms and molecules when excited by laser pulses. We present other, existing computational TDDFT methods that are suitable for the calculation of electron emission in compact spatial regions, and compare their results. We illustrate the performance of the new method by simulating strong-field ionization of C60 fullerene and discuss final state effects in the orbital reconstruction of planar organic molecules.
Levels of self-consistency in the GW approximation
2009
We perform $GW$ calculations on atoms and diatomic molecules at different levels of self-consistency and investigate the effects of self-consistency on total energies, ionization potentials and on particle number conservation. We further propose a partially self-consistent $GW$ scheme in which we keep the correlation part of the self-energy fixed within the self-consistency cycle. This approximation is compared to the fully self-consistent $GW$ results and to the $G W_0$ and the $G_0W_0$ approximations. Total energies, ionization potentials and two-electron removal energies obtained with our partially self-consistent $GW$ approximation are in excellent agreement with fully self-consistent $…
Numerical evidence for a thermal driving force during adsorption of butane in silicalite.
2009
International audience; The transport properties of nano-porous materials determine their applicability, e.g. as separators or catalysts (J. Ka¨rger, D. Ruthven. Diffusion in zeolites, Wiley, New York (1991); L.V.C. Rees, D. Shen. Adsorption of gases in zeolite molecular sieves. In Introduction to Zeolite Science and Practice, Studies in surface science and catalysis, H.V.C. van Bekkum, E.M. Flanigen, P.A. Jacobs, J.C. Jansen (Eds.), vol. 137, pp. 579–631, Elsevier, Amsterdam (2001)). Adsorption in zeolites is explained as a two-step process; adsorption to the external crystal surface and subsequent intra-crystalline diffusion (R. M. Barrer. Porous crystal membranes. J. Chem. Soc. Faraday T…
Functionnalized magnetite nanoparticles for bimodal imaging MRI/PET
2015
Functionalized magnetite nanoparticles for bimodal MRI/PET imagingSuperParamagnetic Iron Oxide Nanoparticles (SPIONs) have been widely studied in the biomedical field due to their promising application as nanodrugs and MRI (Magnetic Resonance Imaging) contrast agents (T2). In this study, magnetite (Fe3O4) nanoparticles have been developed for use as contrast agents for MRI/PET (Positron emission tomography) double imaging. First, functionalized stable superparamagnetic SPIONs have been synthesized in a continuous hydrothermal reactor. During the synthesis, hydrophilic agents (citric acid, LDOPA, DHCA and PHA) have been grafted on the surface of the nanoparticles. The functionalization of th…
Approximate energy functionals for one-body reduced density matrix functional theory from many-body perturbation theory
2018
We develop a systematic approach to construct energy functionals of the one-particle reduced density matrix (1RDM) for equilibrium systems at finite temperature. The starting point of our formulation is the grand potential $\Omega [\mathbf{G}]$ regarded as variational functional of the Green's function $G$ based on diagrammatic many-body perturbation theory and for which we consider either the Klein or Luttinger-Ward form. By restricting the input Green's function to be one-to-one related to a set on one-particle reduced density matrices (1RDM) this functional becomes a functional of the 1RDM. To establish the one-to-one mapping we use that, at any finite temperature and for a given 1RDM $\…
Electronic structure of the ytterbium monohydroxide molecule to search for axionlike particles
2021
Recently, the YbOH molecule has been suggested as a candidate to search for the electron electric dipole moment (eEDM), which violates spatial parity ($P$) and time-reversal ($T$) symmetries [I. Kozyryev and N. R. Hutzler, Phys. Rev. Lett. 119, 133002 (2017)]. In the present paper, we show that the same system can be used to measure coupling constants of the interaction of electrons and nucleus mediated by axionlike particles. The electron-nucleus interaction produced by the axion exchange can contribute to a $T,P$-violating EDM of the whole molecular system. We express the corresponding $T,P$-violating energy shift produced by this effect in terms of the axion mass and product of the axion…