Abstract

All-optical molecular orientation can be realized by applying linearly polarized two-color laser fields [1,2]. This technique can be extended to the three-dimensional molecular orientation with the polarizations of the two-color pulses crossed [3,4]. Recently, we proposed a novel approach to achieve one- and three-dimensional molecular orientation with a linearly polarized fundamental pulse and an elliptically polarized second harmonic pulse, which is advantageous when the molecular orientation dynamics is nonadiabatic [5,6]. In order to explore the dynamics of the three-dimensional molecular orientation, here we solve a time-dependent Schrödinger equation for a linearly polarized fundamental pulse and an elliptically polarized second harmonic pulse, i.e., $E(t)=\left[E_{\omega }(t)\cos (\omega t)+E_{2\omega }(t)\cos (2\omega t+\Phi )\right]\widehat{z}+E_{2\omega }^{\prime }(t)\sin (2\omega t+\Phi \text{) }\widehat{x}$ is applied [5,6].

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