title: First order simultaneous optimization of molecular geometry and electronic wave function.
abstract: 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.
authors.affiliation: Department of Chemistry, University of Washington, Seattle, Washington 98195-1700, USA.
authors.forename: Christopher L
authors.initials: CL
authors.lastname: Moss
authors.forename: Xiaosong
authors.initials: X
authors.lastname: Li