Performant Automatic Differentiation of Local Coupled Cluster Theories: Response Properties and Ab Initio Molecular Dynamics
arxiv(2024)
摘要
In this work, we introduce a differentiable implementation of the local
natural orbital coupled cluster (LNOCC) method within the automatic
differentiation framework of the PySCFAD package. The implementation is
comprehensively tuned for enhanced performance, which enables the calculation
of first-order static response properties on medium-sized molecular systems
using coupled cluster theory with single, double, and perturbative triple
excitations [CCSD(T)]. We evaluate the accuracy of our method by benchmarking
it against the canonical CCSD(T) reference for nuclear gradients, dipole
moments, and geometry optimizations. In addition, we demonstrate the
possibility of property calculations for chemically interesting systems through
the computation of bond orders and Mössbauer spectroscopy parameters for a
[NiFe]-hydrogenase active site model, along with the simulation of infrared
(IR) spectra via ab initio LNO-CC molecular dynamics for a protonated water
hexamer.
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