Using a linearly polarized fundamental pulse and an elliptically polarized second-harmonic pulse, we have recently shown that both all-optical one-dimensional orientation of linear molecules which belong to the point group $C_{\infty \mathrm{v}}$ [Hossain and Sakai, J. Chem. Phys. 153, 104102 (2020)] and three-dimensional orientation of asymmetric-top molecules which belong to the point group $C_2\mathrm{v}$ [Hossain, Esaki, and Sakai, Phys. Rev. A 108, 063109 (2023)] can be achieved. Here, we show that our method can further be extended to realize enantioselective three-dimensional orientation of chiral molecules which belong to the point group $C_1$. Using alanine molecules as a sample, we show that three-dimensional molecular orientation is realized when the relative phase difference between the two wavelengths is not an integer multiple of $\pi /2$. Moreover, the two enantiomers of the alanine molecule are oriented in the opposite directions along the laser propagation direction, indicating that the realized three-dimensional orientation is enantioselective. The advantages of our method, such as robustness and controllability, are discussed.

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• Atomic & molecular processes in external fields
• Light-matter interaction