Controlled quantum-state-resolved chemistry to enable quantum logic with molecular ions
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Controlled quantum-state-resolved chemistry to enable quantum logic with molecular ions


This dissertation describes experiments performed in the MOTion trap, a hybrid atom--ion trap comprised of a magneto-optical trap (MOT) and a linear Paul trap with an integrated time-of-flight mass spectrometer (ToF-MS).We aim to sympathetically cool the vibrational and rotational degrees of freedom of a BaCl$^+$ molecular ion by overlapping a cold ($\sim4$~mK) Ca MOT. This sympathetic cooling can prepare a molecular ion in its rovibrational quantum ground state, providing a method for state preparation for applications in molecular ion quantum logic. While collisions between the molecular ion and the cold atoms can cool the internal degrees of freedom, chemical reactions are also possible for electronically excited atoms. As such, we study these excited-state atom--ion reactions at low temperature $<1$~K and develop tools to control these collisions. We make the first experimental observation of reaction blockading, an effect that suppresses excited-state reactions at low temperature, and develop a method to reverse this suppression if desired with the addition of a catalyst laser, providing a means to optically control such reactions.

Beyond its intended purpose of studying and achieving sympathetic cooling, we find that this apparatus is a powerful tool for chemical studies.By imaging the ions, we can observe reactions occurring one atom at a time. We can precisely tune the collision energy or temperature down to the mK regime to as high as $\sim$10~K using techniques described in this dissertation, allowing controlled interrogation of these low-temperature reactions. Further, using lasers to address electronic transitions, we can precisely control the quantum state of the reactants, and we can measure the reaction products with the ToF-MS. A testament to the value of this apparatus is the study of BaOCa$^+$ described in this dissertation. Using the tools of the MOTion trap, we were able to identify the production of BaOCa$^+$, the first observation of a mixed hypermetallic oxide, and determine the path of reaction as BaOCH$_3^+$ + Ca($4s4p$~$^3P_J$) $\rightarrow$ BaOCa$^+$ + CH$_3$.

In addition to developing control of these atom--ion interactions towards sympathetic cooling of molecular ions, we also work towards further developing new quantum logic schemes for molecular ions, such as dipolar quantum logic, dipole--phonon quantum logic (DPQL), and electric-field gradient gates (EGGs).Specifically, we propose a class of molecules particularly well-suited for DPQL, the alkaline earth monoxide cations, that can also be added to existing atomic ion experiments with minimal additional experimental complexity. We further develop the techniques for DPQL and propose methods for single- and two-qubit gates, outlining a path towards universal quantum computation with molecular ions.

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