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MO: Fachverband Molekülphysik
MO 26: Contributions to SYLC II
MO 26.6: Vortrag
Donnerstag, 5. März 2026, 16:00–16:15, P 110
Optimising enantioselective electronic population transfer in chiral molecules — •Daniel García González and Andrés Ordóñez — Department of Physics, Freie Universität Berlin, Berlin, Germany
Coherent control offers powerful routes to all-optical enantioselective photochemistry. Our approach is based on electronic transitions, requires neither cold molecules nor intermediate resonances nor chiral sensitisers, and is applicable to randomly oriented molecules. Strong (>10%) population differences in opposite enantiomers arise from the interference between two multiphoton excitation pathways driven by a fundamental IR field and two of its harmonics.
In this regime, the population difference takes the form [arXiv:2309.02392v2]
| PR−PS ∝ Re | ⎡ ⎣ | g(5) · h(5) | ⎤ ⎦ | , |
where g(5) encodes the molecular geometry, while h(5) depends on the polarizations of the applied fields and is experimentally controllable.
We study the dependence of g(5) on the molecular structure using the three conformers of carvone, and introduce a strategy to design polarisation schemes that maximise Re[g(5) · h(5)]. This approach yields experimentally realistic field configurations achieving enantioselective population differences of up to 55% -nearly twice the previously reported 30%- offering a clear, geometry-based method for optimising coherent enantioselective control in electronic transitions.
Keywords: chiral molecules; enantioselective control; coherent control; electronic transitions; ultrafast dynamics