From Symmetry Breaking via Charge Migration to Symmetry Restoration in Electronic Ground and Excited States: Quantum Control on the Attosecond Time Scale

Abstract

This article starts with an introductory survey of previous work on breaking and restoring the electronic structure symmetry of atoms and molecules by means of two laser pulses. Accordingly, the first pulse breaks the symmetry of the system in its ground state with irreducible representation IRREPg by exciting it to a superposition of the ground state and an excited state with different IRREPe . The superposition state is non-stationary, representing charge migration with period T in the sub- to few femtosecond time domains. The second pulse stops charge migration and restores symmetry by de-exciting the superposition state back to the ground state. Here, we present a new strategy for symmetry restoration: The second laser pulse excites the superposition state to the excited state, which has the same symmetry as the ground state, but different IRREPe . The success depends on perfect time delay between the laser pulses, with precision of few attoseconds. The new strategy is demonstrated by quantum dynamics simulation for an oriented model system, benzene.