Observation of vibrational overtones by single molecule resonant photodissociation

Abstract

Molecular ions can be held in a chain of laser-cooled atomic ions by sympathetic cooling. This system is ideal for performing high-precision molecular spectroscopy with applications in astrochemistry and fundamental physics. Here we show that this same system can be coupled with a broadband laser to discover new molecular transitions. We use three-ion chains of Ca${}^{+}$ and CaH${}^{+}$ to observe vibrational transitions via resonance enhanced multiphoton dissociation detected by Ca${}^{+}$ fluorescence. Based on theoretical calculations, we assign the observed peaks to the transition from the ground vibrational state, $\nu =0$, to $\nu =9$ and $\nu =10$. Our method allows us to track single molecular events, and it can be extended to work with any molecule by using normal mode frequency shifts to detect the dissociation. This survey spectroscopy serves as a bridge to the precision spectroscopy required for molecular ion control.

11 pages, 3 figures, updated to published version

References in corpus (4)

• Enhanced sensitivity to variation of $m_e/m_p$ in molecular spectra
• Probing isotope effects in chemical reactions using single ions
• Sympathetic cooling of molecular ion motion to the ground state
• Laser-cooling-assisted mass spectrometry

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• Sympathetic cooling of ${}^{40}{\text{Ca}}^{+}$ - ${}^{27}{\text{Al}}^{+}$ ion pair crystal in a linear Paul trap
• Vibronic spectroscopy of sympathetically cooled CaH${}^{+}$
• Prospects for Polar Molecular Ion Optical Probe of Varying Proton-Electron Mass Ratio
• Ultracold ion-atom experiments: cooling, chemistry, and quantum effects
• Reassigning the CaH${}^{+}$ 1${}^1\Sigma \to$ 2${}^1\Sigma$ vibronic transition with CaD${}^{+}$
• Studying fundamental physics using quantum enabled technologies with trapped molecular ions
• Photodissociation spectra of single trapped CaOH+ molecular ions
• Precise Determination of Excited State Rotational Constants and Black-Body Thermometry in Coulomb Crystals of Ca${}^{+}$ and CaH${}^{+}$
• Coulomb crystallization of xenon highly charged ions in a laser-cooled Ca+ matrix