EXIDOS

Variational low-energy subspaces for chemically accurate excited states

Announce Type: new Abstract: Accurate electronic excited states are essential for photochemistry, spectroscopy and non-adiabatic molecular dynamics, but high-level calculations often scale steeply and require prior knowledge of the target state's character or symmetry. Here we show that variational excited-state optimization can be reformulated as an iterated ground-state-like problem for a low-energy subspace of the electronic Hamiltonian. Applying this variational principle to...