Ab initio molecular simulations with numeric atom-centered orbitals

By Volker Blum, Ralf Gehrke, Felix Hanke, Paula Havu, Ville Havu, Xinguo Ren, Karsten Reuter, Matthias Scheffler. 2009

2,594 citations recorded by the source corpus.

We describe a complete set of algorithms for ab initio molecular simulations based on numerically tabulated atom-centered orbitals (NAOs) to capture a wide range of molecular and materials properties from quantum-mechanical first principles. The full algorithmic framework described here is embodied in the Fritz Haber Institute “ab initio molecular simulations” (FHI-aims) computer program package. Its comprehensive description should be relevant to any other first-principles implementation based on NAOs. The focus here is on density-functional theory (DFT) in the local and semilocal (generalized gradient) approximations, but an extension to hybrid functionals, Hartree–Fock theory, and MP2/GW electron self-energies for total energies and excited states is possible within the same underlying algorithms. An all-electron/full-potential treatment that is both computationally efficient and accurate is achieved for periodic and cluster geometries on equal footing, including relaxation and ab initio molecular dynamics. We demonstrate the construction of transferable, hierarchical basis sets, allowing the calculation to range from qualitative tight-binding like accuracy to meV-level total energy convergence with the basis set. Since all basis functions are strictly localized, the otherwise computationally dominant grid-based operations scale as O(N) with system size N. Together with a scalar-relativistic treatment, the basis sets provide access to all elements from light to heavy. Both low-communication parallelization of all real-space grid based algorithms and a ScaLapack-based, customized handling of the linear algebra for all matrix operations are possible, guaranteeing efficient scaling (CPU time and memory) up to massively parallel computer systems with thousands of CPUs.

Subfields: Atomic and Molecular Physics, and Optics, Materials Chemistry

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Citations in the corpus

Deep Potentials for Materials Science (2022, methodology): “Data ﬁles can be written in one of the following package formats: VASP [66, 67], LAMMPS [81], Gaussian [85], SIESTA [86], CP2K [87], QE [68], FHI-aims [88], QUIP [89], PWmat [14, 15], AMBER [90], GROMACS [84], and ABA-CUS [69].”
Reproducibility in density functional theory calculations of solids (2016, methodology): “A third possibility is to use the atomic zero-order regular approximation, as was done in the FHIaims code package (tables S5 to S7) (42, 55).”
Jmol – a paradigm shift in crystallographic visualization (2010, methodology): “Additional file formats of interest within the crystallographic community that are supported include files generated by the programs FHI-aims (Blum et al., 2009; http://www.fhi-berlin. mpg.de/aims), CASTEP (Segall et al., 2002; http://www.castep. org), CRYSTAL (Dovesi et al., 1989), VASP (Jurgen, 20”
Siesta: Recent developments and applications. (2020, methodology): “This is the case of FHI-aims, 13 which uses a more sophisticated real-space grid (atom-centered), thus extending the core scheme to all-electron calculations.”