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An important physical process unique to neutral-ion systems is the charge-transfer (CT) reaction. Here, we present measurements of and models for CT processes between co-trapped ultracold Ca atoms and Yb ions under well-controlled conditions. The theoretical analysis reveals the existence of three reaction mechanisms when lasers from a magneto-optical trap (MOT) and an additional catalyst laser are present. Besides the direct CT involving existent excited Ca population in the MOT, the second pathway is controlled by MOT-induced CT, whereas the third one mostly involves the additional red-detuned laser.

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