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We demonstrate and explore an all-optical technique for direct monitoring theorientation dynamics of gas phase molecular ensembles. The technique termed'MOISH' utilizes the transiently lifted inversion symmetry of polar gas mediaand provides a sensitive and spatially localized probing of second harmonicgeneration signal that is directly correlated with the orientation of the gas.Our experimental results reveal selective electronic and nuclear dynamicalcontributions to the overall nonlinear optical signal and decipher them apartusing the "reporter gas" approach. 'MOISH' provides new, crucial means forexploring controlled rotational dynamics via concerted terahertz and opticalfield excitation.

Molecular Orientation-Induced Second Harmonic Generation: deciphering different contributions apart