We present quantum dynamical simulations for the laser driven isomerization of an ensemble of surface mounted stereoisomers with multiple orientations. The model system 1-(2-cis-fluoroethenyl)-2-fluorobenzene supports two chiral and one achiral atropisomers upon torsion around the C–C single bond connecting phenyl ring and ethylene group. An infrared picosecond pulse is used to excite the internal rotation around the chiral axis, thereby controlling the chirality of the molecule. In order to selectively switch the molecules—independent of their orientation on a surface—from their achiral to either their left- or right-handed form, a stochastic pulse optimization algorithm is applied. The stochastic pulse optimization is performed for different sets of defined orientations of adsorbates corresponding to the rotational symmetry of the surface. The obtained nonlinearly polarized laser pulses are highly enantioselective for each orientation.

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