Hybrid basis and multi-center grid method for strong-field processes

Abstract

We present a time-dependent framework that combines a hybrid Gaussian-FEDVR basis with a multicenter grid to simulate strong-field and attosecond dynamics in atoms and molecules. The method incorporates the construction of the orthonormal hybrid basis, the evaluation of electronic integrals, a unitary time-propagation scheme, and the extraction of optical and photoelectron observables. Its accuracy and robustness are benchmarked on one-electron systems such as atomic hydrogen and the dihydrogen cation ($\text{H}_{2}^{+}$) through comparisons with essentially-exact reference resutls for bound-state energies, high-harmonic generation spcetra, photoionization cross sections, and photoelectron momentum distributions. This work establishes the groundwork for its integration with quantum-chemistry methods, which are already operational but will be detailed in future work, thereby enabling ab initio simulations of correlated polyatomic systems in intense ultrafast laser fields.