Local Pair Natural Orbital-Based Coupled-Cluster Theory through Full Quadruples (DLPNO–CCSDTQ)
Andy Jiang, Devin A. Matthews, David Poole, Connor G. Briggs, Justin M. Turney, C. David Sherrill, Henry F. Schaefer III
TL;DR
This paper introduces a new quantum chemistry method for accurately calculating molecular energies using advanced computational techniques.
Contribution
The novel method extends local pair natural orbital-based coupled-cluster theory to include full quadruples for higher accuracy.
Findings
The method achieves energy differences within 0.01–0.05 kcal mol–1 compared to canonical CCSDTQ.
Computations for complex systems like benzene dimer and adamantane become feasible with this approach.
Abstract
In this work, we implement a local pair natural orbital-based coupled-cluster method through the full treatment of quadruple excitations (CCSDTQ). The domain-based local pair natural orbital (DLPNO) approach, which has successfully been applied to lower levels of coupled-cluster theory, is utilized in our algorithm, and thus our algorithm is called DLPNO-CCSDTQ. For simplicity in the working equations and in the implementation, we t 1-dress the two-electron integrals as well as Fock matrix elements. Our method can recover CCSDTQ-CCSDT and CCSDTQ-CCSDT(Q) energy differences on the order of 0.01–0.05 kcal mol–1, even at a loose quadruples natural orbital (QNO) occupation number cutoff of 3.33 × 10–6. To highlight the capabilities of our code and its potential future applications, we showcase computations that would be intractable with canonical CCSDTQ, such as the benzene dimer, (H2O)17,…
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Taxonomy
TopicsAdvanced Chemical Physics Studies · Magnetism in coordination complexes · Synthesis and Properties of Aromatic Compounds