Improved Optimization for the Cluster Jastrow Antisymmetric Geminal Power and Tests on Triple-Bond Dissociations.
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 N2 and the transition-metal-oxide example of [ScO](+).
Department of Chemistry, University of California , Berkeley, California 94720, United States.|Chemical Science Division, Lawrence Berkeley National Laboratory , Berkeley, California 94720, United States.
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Neuscamman