Reproducibility in density functional theory calculations of solids.

The widespread popularity of density functional theory has given rise to an extensive range of dedicated codes for predicting molecular and crystalline properties. However, each code implements the formalism in a different way, raising questions about the reproducibility of such predictions. We report the results of a community-wide effort that compared 15 solid-state codes, using 40 different potentials or basis set types, to assess the quality of the Perdew-Burke-Ernzerhof equations of state for 71 elemental crystals. We conclude that predictions from recent codes and pseudopotentials agree very well, with pairwise differences that are comparable to those between different high-precision experiments. Older methods, however, have less precise agreement. Our benchmark provides a framework for users and developers to document the precision of new applications and methodological improvements.

Direct fabrication of large micropatterned single crystals.

Micropatterning of single crystals for technological applications is a complex, multistep process. Nature provides alternative fabrication strategies, when crystals with exquisite micro-ornamentation directly develop within preorganized frameworks. We report a bio-inspired approach to growing large micropatterned single crystals. Micropatterned templates organically modified to induce the formation of metastable amorphous calcium carbonate were imprinted with calcite nucleation sites. The template-directed deposition and crystallization of the amorphous phase resulted in the fabrication of millimeter-sized single calcite crystals with sub-10-micron patterns and controlled crystallographic orientation. We suggest that in addition to regulating the shape, micropatterned frameworks act as sites for stress and impurity release during the amorphous-to-crystalline transition. The proposed mechanisms may have direct biological relevance and broad implications in materials synthesis.

Absolute and approximate calculations of electron-energy-loss spectroscopy edge thresholds.

Systematic studies of binding energies for the electron excitation of core levels for atoms, molecules, and solids have been calculated with various density functional theories. The generalized gradient approximation provides the most accurate description of the absolute binding energies when spin polarization is included. Relative core level shifts can be determined to within 0.5 eV without spin polarization. Core level shifts can be predicted from ground-state eigenvalue differences only when comparing environments of similar electronegativity. Such is the case for the O K edge, but not the Si L edge at Si/SiO(2) interfaces in nanotransistors.