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We experimentally study the optical- and terahertz- induced rotationaldynamics of asymmetric molecules in the gas phase. Terahertz and optical fieldsare identified as two distinct control handles over asymmetric molecules, asthey couple to the rotational degrees of freedom via the molecular- dipole andpolarizability selectively. The distinction between those two rotationalhandles is highlighted by different types of quantum revivals observed in longduration (>100ps) field-free rotational evolution. The experimental results arein excellent agreement with Random Phase Wave Function simulations [Phys. Rev.A 91, 063420 (2015)] and provide verification of the RPWF as an efficientmethod for calculating asymmetric molecular dynamics at ambient temperatures,where exact calculation methods are practically not feasible. Our observationsand analysis pave the way for orchestrated excitations by both optical and THzfields as complementary rotational handles, that enable a plethora of newpossibilities in three-dimensional rotational control of asymmetric molecules.

Rotational control of asymmetric molecules: dipole- vs. polarizability- driven rotational dynamics