René Nardi

Absorption spectroscopy is a fundamental tool for probing molecular structure. However, performing absorption spectroscopy on individual molecules is challenging due to the low signal-to-noise ratio. Here, we report on a nondestructive absorption spectroscopy on a mid-infrared vibrational transition in a single molecular ion that is co-trapped with an atomic ion. The absorption of a single photon is detected via the momentum transfer from the absorbed photon onto the molecule. This recoil signal is amplified using a non-classical state of motion of the two-ion crystal and subsequently read out via the atomic ion. We characterize the recoil detection method and use it to investigate the interaction between femtosecond laser pulses and the O-H stretching vibration in individual CaOH+ molecular ions. Furthermore, we present the single-photon absorption spectrum obtained for the vibrational transition. This method represents a milestone towards quantum non-demolition measurements of complex polyatomic molecules, providing high-fidelity methods for preparation and measurement of the quantum state of a wide range of molecular species.

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 $λ=$245 - 275$\,$nm and for two-photon processes at $λ=$500 - 540$\,$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.