No need for a grid: Adaptive fully-flexible gaussians for the time-dependent Schr\"odinger equation

Abstract

Linear combinations of complex gaussian functions, where the linear and nonlinear parameters are allowed to vary, are shown to provide an extremely flexible and effective approach for solving the time-dependent Schr\"odinger equation in one spatial dimension. The use of flexible basis sets has been proven notoriously hard within the systematics of the Dirac--Frenkel variational principle. In this work we present an alternative time-propagation scheme that de-emphasizes optimal parameter evolution but directly targets residual minimization via the method of Rothe's method, also called the method of vertical time layers. We test the scheme using a simple model system mimicking an atom subjected to an extreme laser pulse. Such a pulse produces complicated ionization dynamics of the system. The scheme is shown to perform very well on this model and notably does not rely on a computational grid. Only a handful of gaussian functions are needed to achieve an accuracy on par with a high-resolution, grid-based solver. This paves the way for accurate and affordable solution of the time-dependent Schr\"odinger equation for atoms and molecules within and beyond the Born--Oppenheimer approximation.