7,344 research outputs found
A wavelet-based Projector Augmented-Wave (PAW) method: reaching frozen-core all-electron precision with a systematic, adaptive and localized wavelet basis set
We present a Projector Augmented-Wave~(PAW) method based on a wavelet basis
set. We implemented our wavelet-PAW method as a PAW library in the ABINIT
package [http://www.abinit.org] and into BigDFT [http://www.bigdft.org]. We
test our implementation in prototypical systems to illustrate the potential
usage of our code. By using the wavelet-PAW method, we can simulate charged and
special boundary condition systems with frozen-core all-electron precision.
Furthermore, our work paves the way to large-scale and potentially order-N
simulations within a PAW method
The hiphive package for the extraction of high-order force constants by machine learning
The efficient extraction of force constants (FCs) is crucial for the analysis
of many thermodynamic materials properties. Approaches based on the systematic
enumeration of finite differences scale poorly with system size and can rarely
extend beyond third order when input data is obtained from first-principles
calculations. Methods based on parameter fitting in the spirit of interatomic
potentials, on the other hand, can extract FC parameters from semi-random
configurations of high information density and advanced regularized regression
methods can recover physical solutions from a limited amount of data. Here, we
present the hiPhive Python package, that enables the construction of force
constant models up to arbitrary order. hiPhive exploits crystal symmetries to
reduce the number of free parameters and then employs advanced machine learning
algorithms to extract the force constants. Depending on the problem at hand
both over and underdetermined systems are handled efficiently. The FCs can be
subsequently analyzed directly and or be used to carry out e.g., molecular
dynamics simulations. The utility of this approach is demonstrated via several
examples including ideal and defective monolayers of MoS as well as bulk
nickel
Wavefunction-based correlated ab initio calculations on crystalline solids
We present a wavefunction-based approach to correlated ab initio calculations
on crystalline insulators of infinite extent. It uses the representation of the
occupied and the unoccupied (virtual) single-particle states of the infinite
solid in terms of Wannier functions. Electron correlation effects are evaluated
by considering virtual excitations from a small region in and around the
reference cell, keeping the electrons of the rest of the infinite crystal
frozen at the Hartree-Fock level. The method is applied to study the ground
state properties of the LiH crystal, and is shown to yield rapidly convergent
results.Comment: 6 pages, RevTex, to appear in Phys. Rev.
Charge Transport through Polyene Self-Assembled Monolayers from Multiscale Computer Simulations
We combine first-principles density-functional theory with matrix Green’s function calculations to predict the structures and charge transport characteristics of self-assembled monolayers (SAMs) of four classes of systems in contact with Au(111) electrodes: conjugated polyene chains (n = 4, 8, 12, 16, and 30) thiolated at one or both ends and saturated alkane chains (n = 4, 8, 12, and 16) thiolated at one or both ends. For the polyene SAMs, we find no decay in the current as a function of chain length and conclude that these 1−3 nm long polyene SAMs act as metallic wires. We also find that the polyene-monothiolate leads to a contact resistance only 2.8 times higher than that for the polyene-dithiolate chains, indicating that the device conductance is dominated by the properties of the molecular connector with less importance in having a second molecule−electrode contact. For the alkane SAMs, we observe the normal exponential decay in the current as a function of the chain length with a decay constant of βn = 0.82 for the alkane-monothiolate and 0.88 for the alkane-dithiolate. We find that the contact resistance for the alkane-monothiolate is 12.5 times higher than that for the alkane-dithiolate chains, reflecting the extra resistance due to the weak contact on the nonthiolated end. These contrasting charge transport characteristics of alkane and polyene SAMs and their contact dependence are explained in terms of the atomic projected density of states
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