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 C2Π 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.
Highlights
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
The rotational state distributions were maintained by optical pumping for 10–20 min, limited only by chemical reaction with background H2
Molecular structure at high energies determines the long-range forces which play a crucial role in dissociation and reaction dynamics, for example determining the stability and lifetimes of reactive complexes
Summary
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. Super rotors have been produced by chirped high-intensity fields in optical centrifuges, where the dynamics are understood as response to a classical “corkscrew” potential or alternately as from a sequence of Raman transitions[2] While this is a very elegant approach which works for a broad class of molecules, the Liouville theorem implies that without dissipation, entropy cannot be reduced. They are initially rotationally hot, and pumping narrows the entire distribution to a few rotational levels about the target We use these narrow ensembles of super rotors to probe molecular structure far from the equilibrium bond length and to perform spectroscopy of a previously unobserved excited electronic state
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