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  1. ; ; ; ; ; ; (, Nature Communications)
    Abstract Optical pumping of molecules provides unique opportunities for control of chemical reactions at a wide range of rotational energies. This work reports a chemical reaction with extreme rotational excitation of a reactant and its kinetic characterization. We investigate the chemical reactivity for the hydrogen abstraction reaction SiO++ H2 → SiOH++ H in an ion trap. The SiO+cations are prepared in a narrow rotational state distribution, including super-rotor states with rotational quantum number (j) as high as 170, using a broad-band optical pumping method. We show that the super-rotor states of SiO+substantially enhance the reaction rate, a trend reproduced by complementary theoretical studies. We reveal the mechanism for the rotational enhancement of the reactivity to be a strong coupling of the SiO+rotational mode with the reaction coordinate at the transition state on the dominant dynamical pathway. 
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  2. ; ; (, Physical Review A)
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  3. ; ; ; ; ; (, Nature Communications)
    null (Ed.)
    Abstract Improved optical control of molecular quantum states promises new applications including chemistry in the quantum regime, precision tests of fundamental physics, and quantum information processing. While much work has sought to prepare ground state molecules, excited states are also of interest. Here, we demonstrate a broadband optical approach to pump trapped SiO + molecules into pure super rotor ensembles maintained for many minutes. Super rotor ensembles pumped up to rotational state N  = 67, corresponding to the peak of a 9400 K distribution, had a narrow N spread comparable to that of a few-kelvin sample, and were used for spectroscopy of the previously unobserved C 2 Π state. Significant centrifugal distortion of super rotors pumped up to N  = 230 allowed probing electronic structure of SiO + stretched far from its equilibrium bond length. 
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  4. ; ; ; ; (, Physical Review Letters)
    null (Ed.)
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