All-optical field-free three-dimensional orientation of asymmetric-top molecules

• DOI: 10.1038/s41467-018-07567-2
• Publication Date: 2018-11-27T15:42:16Z
• Authors: Kang Lin; Ilia Tutunnikov; Junjie Qiang; Junyang Ma; Qiying Song; Qinying Ji; Wenbin Zhang; Hanxiao Li; Fenghao Sun; Xiaochun Gong; Hui Li; Peifen Lu; Heping Zeng; Yehiam Prior; Ilya Sh. Averbukh; Jian Wu
• Keywords: Chemical Physics (physics.chem-ph); Science; Physics - Chemical Physics; Q; 0103 physical sciences; FOS: Physical sciences; 01 natural sciences; Article; Physics - Optics; Optics (physics.optics)

AbstractOrientation and alignment of molecules by ultrashort laser pulses is crucial for a variety of applications and has long been of interest in physics and chemistry, with the special emphasis on stereodynamics in chemical reactions and molecular orbitals imaging. As compared to the laser-induced molecular alignment, which has been extensively studied and demonstrated, achieving molecular orientation is a much more challenging task, especially in the case of asymmetric-top molecules. Here, we report the experimental demonstration of all-optical field-free three-dimensional orientation of asymmetric-top molecules by means of phase-locked cross-polarized two-color laser pulse. This approach is based on nonlinear optical mixing process caused by the off-diagonal elements of the molecular hyperpolarizability tensor. It is demonstrated on SO2 molecules and is applicable to a variety of complex nonlinear molecules.