Complete Controllability Despite Degeneracy: Quantum Control of Enantiomer-Specific State Transfer in Chiral Molecules

Understand

We prove complete controllability for rotational states of an asymmetric top molecule belonging to degenerate values of the orientational quantum number M.

• Based on this insight, we construct a pulse sequence that energetically separates population initially distributed over degenerate M-states, as a precursor for orientational purification.
• Introducing the concept of enantio-selective controllability, we determine the conditions for complete enantiomer-specific population transfer in chiral molecules and construct pulse sequences realizing this transfer for population initially distributed over degenerate M-states.
• This degeneracy presently limits enantiomer-selectivity for any initial state except the rotational ground state.