With this background in mind, in the present paper, we have three goals in mind. First, because the molecular constraint just described above [(i)] is highly non-standard, we will show how to derive the necessary equations (and we will further analyze other possible constraints). Second, for the sake of completeness, we will then provide step-by-step instructions delineating exactly how to solve the equations just described, and we will benchmark the convergence of our proposed optimization. Third and finally, going beyond Ref. 48, we will investigate the couplings to the bath that arise from the infinite continuum of states. These couplings are needed if we wish to run fully nonadiabatic dynamics that are compatible with Marcus's electrochemical rate expression and achieve electronic equilibration to the correct temperature, e.g. as in the FSSH-ER dynamics.