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A self-consistent optimally tuned range-separated hybrid density functional (scOT-RSH) approach is developed. It can simultaneously predict accurate geometries, vibrational modes, and frontier orbital energies. This is achieved by optimizing the range-separation parameter, γ, to both satisfy the ionization energy theorem and minimize interatomic forces. We benchmark our approach against an established hybrid functional, B3LYP, using the G2 test set. scOT-RSH greatly improves the accuracy of occupied frontier orbital energies, with a mean absolute error (MAE) of only 0.2 eV relative to experimental ionization energies compared to 2.96 eV with B3LYP. Geometries do not change significantly compared to those obtained from B3LYP, with a bond length MAE of 0.012 Å compared to 0.008 Å for B3LYP, and a 6.5% MAE for zero-point energies, slightly larger than that of B3LYP (3.1%). scOT-RSH represents a new …