Photodissociation spectra of single trapped CaOH+ molecular ions
Abstract: Molecular ions that are generated by chemical reactions with trapped atomic ions can serve as an accessible testbed for developing molecular quantum technologies. On the other hand, they are also a hindrance to scaling up quantum computers based on atomic ions as unavoidable reactions with background gas destroy the information carriers. Here, we investigate the single- and two-photon dissociation processes of single $\text{CaOH}+$ molecular ions co-trapped in $\text{Ca}+$ ion crystals using a femtosecond laser system. We report the photodissociation cross section spectra of $\text{CaOH}+$ for single-photon processes at $\lambda=$245 - 275$\,$nm and for two-photon processes at $\lambda=$500 - 540$\,$nm. Measurements are interpreted with quantum-chemical calculations, which predict the photodissociation threshold for $\text{CaOH}+\to \text{Ca}++\text{OH}$ at 265$\,$nm. This result can serve as a basis for dissociation-based spectroscopy for studying the internal structure of $\text{CaOH}+$. The result also gives a prescription for recycling $\text{Ca}+$ ions in large-scale trapped $\text{Ca}+$ quantum experiments from undesired $\text{CaOH}+$ ions formed in the presence of background water vapor.
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