Real-Time Simulations of Molecules in Electric Fields via Configuration Interaction Theory

The Time-Dependent Configuration Interaction method (TDCI) propagates the time-dependent electronic wave function in the basis of eigenstates of the time-independent Hamiltonian. Real-time time-dependent methods avoid the complications of commonly employed frequency-domain methods based on time-dependent perturbation theory (i.e. response theory), and the "spectral" (or "parameterized") approach taken in TDCI is particularly well suited to ad-hoc modifications to include additional physics. Inclusion of relativistic spin-orbit coupling and coupling to external electromagnetic fields and cavity photons are a few examples of the flexibility afforded by TDCI. An overview of developments in TDCI is discussed, allowing for novel applications in the quantum control of transition metal species and cavity quantum electrodynamics.