In the past few years, the generalized pseudospectral (GPS) method, which is also known as the semispectral method or collocation method, has been successfully applied to investigate the structural properties of atomic and molecular systems,[1–5] the quantum scattering processes in nuclear and atomic physics,[6,7] and the laser-atom interactions.[8–10] Its usefulness has been continuously revealed in recent years in accurately and efficiently solving both the time-independent and time-dependent Schrödinger and Dirac equations. Being a type of discrete variable representation (DVR) method, the GPS method shows its special superiority over other generalizations of DVR, such as the finite difference and finite element methods. For example, the Numerov and Runge-Kutta methods, as in the latter case, are local approaches to the unknown function by a sequence of overlapping low-order polynomials in a small subset of user-defined grid points.[11,12] The GPS method and its variants in different forms are generally global approaches to the unknown function using global basis functions with a high degree, for example, the trigonometric functions or the orthogonal polynomials of a Sturm-Liouville problem.