Global and local optimization of auxiliary basis sets for RI-MP2 calculations
文献信息
Rungtiva Palangsuntikul, Robert Polly, Bernd Hartke
Optimization approaches using several global and local algorithms (genetic algorithms, direct search and implicit filtering) in the search for a global minimum are applied to optimize auxiliary basis sets for quantum chemistry ab initio calculations. We optimize mixed Poisson and density auxiliary basis sets for RI-MP2, by minimizing a suitable objective function ΔI. For H, B, C, N, O and F optimized auxiliary basis sets are reported for cc-pVXZ (X = D, T and Q). The auxiliary basis sets optimized in this work are all even-tempered series. As results from these approaches, we never observed errors (ΔI/|EMP2|) greater than 0.55 μEh per atom. In more than 90% of all cases the errors were smaller than 0.009 μEh. Moreover, these approximations affect molecular MP2 energies by less than 30 μEh per atom. In contrast to traditional attempts to optimize auxiliary basis sets, this approach is faster and more reliable.
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Physical Chemistry Chemical Physics

Physical Chemistry Chemical Physics (PCCP) is an international journal co-owned by 19 physical chemistry and physics societies from around the world. This journal publishes original, cutting-edge research in physical chemistry, chemical physics and biophysical chemistry. To be suitable for publication in PCCP, articles must include significant innovation and/or insight into physical chemistry; this is the most important criterion that reviewers and Editors will judge against when evaluating submissions. The journal has a broad scope and welcomes contributions spanning experiment, theory, computation and data science. Topical coverage includes spectroscopy, dynamics, kinetics, statistical mechanics, thermodynamics, electrochemistry, catalysis, surface science, quantum mechanics, quantum computing and machine learning. Interdisciplinary research areas such as polymers and soft matter, materials, nanoscience, energy, surfaces/interfaces, and biophysical chemistry are welcomed if they demonstrate significant innovation and/or insight into physical chemistry. Joined experimental/theoretical studies are particularly appreciated when complementary and based on up-to-date approaches.











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