Moss Christopher L, Li Xiaosong
Department of Chemistry, University of Washington, Seattle, Washington 98195-1700, USA.
J Chem Phys. 2008 Sep 21;129(11):114102. doi: 10.1063/1.2977735.
We present a very efficient simultaneous optimization method for both molecular geometry and electronic wave function. We introduce a simultaneous least squares scheme to minimize errors in a full local quadratic space of both geometric and wave function vectors. Several self-consistent-field iterations are taken until a uniform search direction is achieved in every geometry optimization step. Not only does this new simultaneous optimization method significantly reduce the number of self-consistent-field iterations to reach convergence, it is able to overcome shallow potential wells to find a better stationary point. This new method exhibits up to approximately 60% savings in computational cost compared to conventional geometry optimization methods.
