Performant automatic differentiation of local coupled cluster theories: Response properties and ab initio molecular dynamics

This work was primarily supported by the United States Department of Energy, Office of Science, Basic Energy Sciences, Chemical Sciences, Geosciences, and Biosciences Division, FWP LANLE3F2 awarded to Los Alamos National Laboratory under Triad National Security, LLC (“Triad”) contract Grant No. 89233218CNA000001, subaward C2448 to the California Institute of Technology. Additional support for G.K.C. was provided by the Camille and Henry Dreyfus Foundation via a grant from the program “Machine Learning in the Chemical Sciences and Engineering.” Some of the calculations were performed at the National Energy Research Scientific Computing Center (NERSC), a U.S. Department of Energy, Office of Science User Facility located at the Lawrence Berkeley National Laboratory.

X.Z. and C.L. contributed equally to this work. X.Z., C.L., and G.K.-L.C. designed this project. H.-Z.Y. and T.C.B. contributed to the original implementation of the LNO-CC method, based on which X.Z. developed the differentiable version used here. H.-Z.Y. and T.C.B. also provided help and advice with the methodology development in the early part of the project. C.L. developed the AIMD simulation workflow. X.Z. and C.L. performed the calculations and wrote the original draft. X.Z., C.L., and G.K.-L.C. validated the data, and all contributed to the reviewing and editing of the manuscript.

Xing Zhang: Conceptualization (equal); Methodology (equal); Software (equal); Validation (equal); Writing – original draft (equal); Writing – review & editing (equal). Chenghan Li: Conceptualization (equal); Methodology (equal); Software (equal); Validation (equal); Writing – original draft (equal); Writing – review & editing (equal). Hong-Zhou Ye: Methodology (supporting); Software (equal); Writing – review & editing (equal). Timothy C. Berkelbach: Methodology (supporting); Writing – review & editing (equal). Garnet Kin-Lic Chan: Conceptualization (equal); Funding acquisition (lead); Supervision (lead); Writing – review & editing (equal).

Additional implementation details and computational results supporting the findings in this work are provided in the supplementary material.