Improved Optimization for the Cluster Jastrow Antisymmetric Geminal Power and Tests on Triple-Bond Dissociations

摘要

We present a novel specialization of the variational Monte Carlo linear method for the optimization of the recently introduced cluster Jastrow antisymmetric geminal power ansatz, achieving a lower-order polynomial cost scaling than would be possible with a naive application of the linear method and greatly improving optimization performance relative to that of the previously employed quasi-Newton approach. We test the methodology on highly multireference triple-bond stretches, achieving accuracy superior to those of the traditional coupled cluster theory and multireference perturbation theory in both the typical example of N-2 and the transition-metal-oxide example of [ScO](+).