التفاصيل البيبلوغرافية
| العنوان: |
Accurate and efficient open-source implementation of domain-based local pair natural orbital (DLPNO) coupled-cluster theory using a t1-transformed Hamiltonian. |
| المؤلفون: |
Jiang, Andy1 (AUTHOR) ajiang10224@gmail.com, Glick, Zachary L.2 (AUTHOR), Poole, David2 (AUTHOR), Turney, Justin M.1 (AUTHOR) justin.turney@uga.edu, Sherrill, C. David2 (AUTHOR) sherrill@gatech.edu, Schaefer III, Henry F.1 (AUTHOR) |
| المصدر: |
Journal of Chemical Physics. 8/28/2024, Vol. 161 Issue 8, p1-20. 20p. |
| مصطلحات موضوعية: |
*COUPLED-cluster theory, *NATURAL orbitals, *WATER clusters, *ORBITAL interaction, *KILLER whale |
| مستخلص: |
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). [ABSTRACT FROM AUTHOR] |
| قاعدة البيانات: |
Academic Search Index |