Related papers: Material specific optimization of Gaussian basis s…
We present an approach for generating local numerical basis sets of improving accuracy for first-principles nanoplasmonics simulations within time-dependent density functional theory. The method is demonstrated for copper, silver, and gold…
First-principles density functional theory (DFT) codes which employ a localized basis offer advantages over those which use plane-wave bases, such as better scaling with system size and better suitability to low-dimensional systems. The…
The projection of the eigenfunctions obtained in standard plane-wave first-principle calculations is used for analyzing atomic-orbital basis sets. The "spilling" defining the error in such a projection allows the evaluation of the quality…
We propose a unique scheme to construct fully optimized atomic basis sets for density-functional calculations. The shapes of the radial functions are optimized by minimizing the {\it spillage} of the wave functions between the atomic…
We present a simple, robust and black-box approach to the implementation and use of local, periodic, atom-centered Gaussian basis functions within a plane wave code, in a computationally efficient manner. The procedure outlined is based on…
The performance of basis sets made of numerical atomic orbitals is explored in density-functional calculations of solids and molecules. With the aim of optimizing basis quality while maintaining strict localization of the orbitals, as…
We introduce a mixed density fitting scheme that uses both a Gaussian and a plane-wave fitting basis to accurately evaluate electron repulsion integrals in crystalline systems. We use this scheme to enable efficient all-electron Gaussian…
A general procedure for the optimization of atomic density-fitting basis functions is designed with the balance between accuracy and numerical stability in mind. Given one-electron wavefunctions and energies, weights are assigned to the…
We present a $GW$ space-time algorithm for periodic systems in a Gaussian basis including spin-orbit coupling. We employ lattice summation to compute the irreducible density response and the self-energy, while we employ $k$-point sampling…
The rapidly growing interest in simulating condensed-phase materials using quantum chemistry methods calls for a library of high-quality Gaussian basis sets suitable for periodic calculations. Unfortunately, most standard Gaussian basis…
We present a quasiparticle self-consistent $GW$ (QSGW) implementation for periodic systems based on crystalline Gaussian basis sets. Our QSGW approach is based on a full-frequency analytic continuation GW scheme with Brillouin zone sampling…
The input of almost every machine learning algorithm targeting the properties of matter at the atomic scale involves a transformation of the list of Cartesian atomic coordinates into a more symmetric representation. Many of the most popular…
Despite the fact that most quantum chemistry basis sets are designed for accurately modelling valence chemistry, these general-purpose basis sets continue to be widely used to model core-dependent properties. Core-specialised basis sets are…
We present the sliding basis computational framework to automatically synthesize heterogeneous (graded or discrete) material fields for parts designed using constrained optimization. Our framework uses the fact that any spatially varying…
A simple yet general method for constructing basis sets for molecular electronic structure calculations is presented. These basis sets consist of atomic natural orbitals from a multi-configurational self-consistent field calculation…
We introduce Bayesian optimization, a technique developed for optimizing time-consuming engineering simulations and for fitting machine learning models on large datasets. Bayesian optimization guides the choice of experiments during…
A few recent works explored incorporating geometric priors to regularize the optimization of Gaussian splatting, further improving its performance. However, those early studies mainly focused on the use of low-order geometric priors (e.g.,…
A systematic method for optimal design of layered periodic composites for mitigation of impact-induced shock waves is presented. Frequency spectrum of a pulse with a sharp rise-time is analyzed and the frequency range that carries most of…
There is growing interest in engineering unconventional computing devices that leverage the intrinsic dynamics of physical substrates to perform fast and energy-efficient computations. Granular metamaterials are one such substrate that has…
Basis sets of atomic orbitals are very efficient for density functional calculations but lack a systematic variational convergence. We present a variational method to optimize numerical atomic orbitals using a single parameter to control…