ABSTRACT We present a deterministic all‐parameter optimization method based on analytic derivatives for vibrational wave functions in a separable product form represented in a distributed Gaussian basis. The optimization of the center and width parameters of the basis allows for compact wave function representations at a small basis size. We illustrate the approach by computing ground and excited vibrational states of anharmonic model systems and the 9‐dimensional formic acid monomer.
Kelemen et al. (Sun,) studied this question.