2,732 research outputs found
Continuum variational and diffusion quantum Monte Carlo calculations
This topical review describes the methodology of continuum variational and
diffusion quantum Monte Carlo calculations. These stochastic methods are based
on many-body wave functions and are capable of achieving very high accuracy.
The algorithms are intrinsically parallel and well-suited to petascale
computers, and the computational cost scales as a polynomial of the number of
particles. A guide to the systems and topics which have been investigated using
these methods is given. The bulk of the article is devoted to an overview of
the basic quantum Monte Carlo methods, the forms and optimisation of wave
functions, performing calculations within periodic boundary conditions, using
pseudopotentials, excited-state calculations, sources of calculational
inaccuracy, and calculating energy differences and forces
Predicting second virial coefficients of organic and inorganic compounds using Gaussian process regression
We show that by using intuitive and accessible molecular features it is possible to predict the temperature-dependent second virial coefficient of organic and inorganic compounds with Gaussian process regression. In particular, we built a low dimensional representation of features based on intrinsic molecular properties, topology and physical properties relevant for the characterization of molecule-molecule interactions. The featurization was used to predict second virial coefficients in the interpolative regime with a relative error ≲1% and to extrapolate the prediction to temperatures outside of the training range for each compound in the dataset with a relative error of 2.1%. Additionally, the model's predictive abilities were extended to organic molecules unseen in the training process, yielding a prediction with a relative error of 2.7%. Test molecules must be well-represented in the training set by instances of their families, which are high in variety. The method shows a generally better performance when compared to several semi-empirical procedures employed in the prediction of the quantity. Therefore, apart from being robust, the present Gaussian process regression model is extensible to a variety of organic and inorganic compounds
On the formation of van der Waals complexes through three-body recombination
In this work, we show that van der Waals molecules X–RG (where RG is the rare gas atom) may be created through direct three-body recombination collisions, i.e., X + RG + RG → X–RG + RG. In particular, the three-body recombination rate at temperatures relevant for buffer gas cell experiments is calculated via a classical trajectory method in hyperspherical coordinates [Pérez-Ríos et al., J. Chem. Phys. 140, 044307 (2014)]. As a result, it is found that the formation of van der Waals molecules in buffer gas cells (1 K ≲ T ≲ 10 K) is dominated by the long-range tail (distances larger than the LeRoy radius) of the X–RG interaction. For higher temperatures, the short-range region of the potential becomes more significant. Moreover, we notice that the rate of formation of van der Walls molecules is of the same order of the magnitude independent of the chemical properties of X. As a consequence, almost any X–RG molecule may be created and observed in a buffer gas cell under proper conditions
Classical threshold law for the formation of van der Waals molecules
We study the role of pairwise long-range interactions in the formation of van der Waals molecules through direct three-body recombination processes A + B + B → AB + B, based on a classical trajectory method in hyperspherical coordinates developed in our earlier works [J. Pérez-Ríos et al., J. Chem. Phys. 140, 044307 (2014); M. Mirahmadi and J. Pérez-Ríos, J. Chem. Phys. 154, 034305 (2021)]. In particular, we find the effective long-range potential in hyperspherical coordinates with an exact expression in terms of dispersion coefficients of pairwise potentials. Exploiting this relation, we derive a classical threshold law for the total cross section and the three-body recombination rate yielding an analytical expression for the three-body recombination rate as a function of the pairwise long-range coefficients of the involved partners
Trajectory-dependent energy loss for swift He atoms axially scattered off a silver surface
Angle- and energy-loss- resolved distributions of helium atoms grazingly
scattered from a Ag(110) surface along low indexed crystallographic directions
are investigated considering impact energies in the few keV range. Final
projectile distributions are evaluated within a semi-classical formalism that
includes dissipative effects due to electron-hole excitations through a
friction force. For mono-energetic beams impinging along the ,
and directions, the model predicts the presence of
multiple peak structures in energy-loss spectra. Such structures provide
detailed information about the trajectory-dependent energy loss. However, when
the experimental dispersion of the incident beam is taken into account, these
energy-loss peaks are completely washed out, giving rise to a smooth
energy-loss distribution, in fairly good agreement with available experimental
data
Energetics of intrinsic point defects in ZrSiO
Using first principles calculations we have studied the formation energies,
electron and hole affinities, and electronic levels of intrinsic point defects
in zircon. The atomic structures of charged interstitials, vacancies, Frenkel
pairs and anti-site defects are obtained. The limit of high concentration of
point defects, relevant for the use of this material in nuclear waste
immobilization, was studied with a variable lattice relaxation that can
simulate the swelling induced by radiation damage. The limit of low
concentration of defects is simulated with larger cells and fixed lattice
parameters. Using known band offset values at the interface of zircon with
silicon, we analyze the foreseeable effect of the defects on the electronic
properties of zircon used as gate in metal-oxide-semiconductor devices.Comment: preprint 16 pages, 4 figures, and 5 table
Ion-atom-atom three-body recombination in cold hydrogen and deuterium plasmas
We present a detailed study about ion-atom-atom three-body recombination in hydrogen and deuterium plasmas based on classical trajectory calculations in hyperspherical coordinates. Our results, due to the predominant role of the long-range charged-induced dipole interaction, indicate that H2+ and D2+ are the main reaction products in the case of hydrogen and deuterium plasmas, respectively. In addition, we find a more steep energy-dependent reaction rate when the collision energy surpasses the dissociation energy of the molecular ion, thus entering a new dynamical regime dominated by short-range interactions
Quantum Monte Carlo study of a positron in an electron gas
Quantum Monte Carlo calculations of the relaxation energy, pair-correlation function, and annihilating-pair momentum density are presented for a positron immersed in a homogeneous electron gas. We find smaller relaxation energies and contact pair-correlation functions in the important low-density regime than predicted by earlier studies. Our annihilating-pair momentum densities have almost zero weight above the Fermi momentum due to the cancellation of electron-electron and electron-positron correlation effects
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