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Long-lasting Molecular Orientation Induced by a Single Terahertz Pulse

Control of molecular rotations by laser fields is an active area of research focusing on the alignment/orientation of otherwise isotropic molecular samples. Oriented molecules are useful in many applications, such as molecular orbital tomography, femtosecond imaging of molecular structure, dynamics and chemical reaction control. In this work, we present a novel, previously unreported phenomenon appearing in thermal ensembles of non-linear polar molecules excited by a single THz pulse. We find that the induced orientation lasts long after the excitation pulse is over. In the case of symmetric-top molecules, the ensemble averaged orientation remains indefinitely constant after the pulse, whereas in the case of asymmetric-top molecules the orientation persists for a long time after the end of the pulse. We discuss the underlying mechanism, study its non-monotonous temperature dependence, and show that there exists an optimal temperature for the maximal residual orientation. The persistent orientation implies long lasting macroscopic dipole moment, which may be probed by second (or higher order) harmonic generation.