Property-optimized gaussian basis sets for molecular response calculations.

摘要: With recent advances in electronic structure methods, first-principles calculations of response properties, such as linear and nonlinear polarizabilities, have become possible for molecules with more than 100 atoms. Basis set incompleteness is typically the main source error since traditional diffuse augmented basis sets are too costly to use or suffer from near dependence. To address this problem, we construct first comprehensive property-optimized elements H–Rn except lanthanides. The new build on Karlsruhe segmented contracted split-valence quadruple-zeta valence quality add a small number moderately functions. exponents determined variationally by maximization atomic Hartree–Fock polarizabilities using analytical derivative methods. performance resulting assessed 313 molecular static polarizabilities. mean...