Car-Parrinello (CP) molecular dynamics [1] is an efficient scheme for classical molecular dynamics (MD) where the interaction potential is defined by a variational principle. The originally proposed combination with the Kohn-Sham (KS) density functional method proved to be most successful, but the CP method has also been applied to other energy functions. [2][3][4] Within the KS method, the plane-wave/pseudopotential framework, also applied in the original paper by Car and Parrinello, remains the most popular. However, recent progress with local-