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We present an efficient, open-source formulation for coupled-cluster theory through perturbative triples with domain-based local pair natural orbitals [DLPNO-CCSD(T)]. Similar to the implementation of the DLPNO-CCSD(T) method found in the ORCA package, the most expensive integral generation and contraction steps associated with the CCSD(T) method are linear-scaling. In this work, we show that the t1-transformed Hamiltonian allows for a less complex algorithm when evaluating the local CCSD(T) energy without compromising efficiency or accuracy. Our algorithm yields sub-kJ mol−1 deviations for relative energies when compared with canonical CCSD(T), with typical errors being on the order of 0.1 kcal mol−1, using our TightPNO parameters. We extensively tested and optimized our algorithm and parameters for non-covalent interactions, which have been the most difficult interaction to model for orbital (PNO)-based methods historically. To highlight the capabilities of our code, we tested it on large water clusters, as well as insulin (787 atoms).more » « less
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Kazemi, Seyed Mehran; Kimmig, Angelika; Van den Broeck, Guy; Poole, David (, Advances in Neural Information Processing Systems 29 (NIPS))
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Barca, Giuseppe M.; Bertoni, Colleen; Carrington, Laura; Datta, Dipayan; De Silva, Nuwan; Deustua, J. Emiliano; Fedorov, Dmitri G.; Gour, Jeffrey R.; Gunina, Anastasia O.; Guidez, Emilie; et al (, The Journal of Chemical Physics)
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