Using the all-optical molecular orientation technique with intense nonresonant two-color laser pulses, stronger molecular orientation |⟨cos θ2D⟩| ∼ 0.34 is achieved by employing the following two strategies: (1) carbonyl sulfide molecules lying in the lower rotational states are selected using a home-built molecular deflector and (2) the rising parts of the two wavelengths of the pump pulse are adjusted by introducing a Michelson-type delay line in the optical path. The achieved degree of molecular orientation is higher than that observed in the proof-of-principle experiment [Oda et al., Phys. Rev. Lett. 104, 213901 (2010)] by about an order of magnitude and the highest ever characterized directly by Coulomb explosion imaging with appropriate probe polarization.

We show that a combination of a fundamental pulse with linear polarization along the vertical direction and an elliptically polarized second harmonic pulse with both vertical and horizontal electric field components can be used to orient linear molecules efficiently, leading to higher degrees of orientation. Due to this specific combination of polarizations, the asymmetric hyperpolarizability interaction potential, which remains the same as that in a linearly polarized two-color laser field, is created along the vertical component of the elliptically polarized second harmonic pulse. On the other hand, the horizontal component suppresses the otherwise strong symmetric polarizability potential responsible for alignment, increasing the tunneling probability from the shallower potential well to the deeper one. As a result, the degree of orientation increases and can be controlled by changing the intensity of the horizontal component of the elliptically polarized second harmonic pulse. This study is the generalization of the all-optical molecular orientation technique based on the anisotropic hyperpolarizability interaction.

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