Coupled Cluster Amplitude Extrapolation in Geometry Optimization
Jonas Beck, Michele Nottoli, Tommaso Nottoli, Luca Melega, Filippo Lipparini, Benjamin Stamm
Abstract
In this work, we present an amplitude extrapolation ansatz for geometry optimization that uses calculations from previous steps to construct an initial guess for the quasi-Newton solver at each new geometry, significantly accelerating convergence of the coupled-cluster and Lambda solver alike. The ansatz incorporates a necessary amplitude transformation to mitigate discontinuities associated with orbital energy crossings at the Hartree-Fock level of theory, while remaining computational and memory efficient. The method is tested for a diverse set of medium-sized molecules to demonstrate a systematic and significant reduction in the number of coupled-cluster iterations compared to the conventional method.
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