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Optical pumping of molecules provides unique opportunities for the control ofchemical reactions at a wide range of rotational energies. Chemical reactivityfor the hydrogen abstraction reaction SiO$^+$ + H$_2$ $\rightarrow$ SiOH$^+$ +H is investigated in an ion trap. The SiO$^+$ cation is prepared with a narrowrotational state distribution, including super-rotor states with rotationalquantum number $\it{(j)}$ as high as 170 using a broad-band optical pumpingmethod. The super-rotor states of SiO$^+$ are shown to substantially enhancethe reaction rate, a trend reproduced by complementary theoretical studies. Themechanism for the rotational enhancement of the reactivity is revealed to be astrong coupling of the SiO$^+$ rotational mode with the reaction coordinate atthe transition state on the dominant dynamical pathway. This work reports forthe first time a chemical reaction with extreme rotational excitation of areactant and its kinetic characterization.

Rotational control of reactivity: Reaction of SiO$^+$ ions in extreme rotational states