Fabian Schmid

We report on efficient rovibrational state-selective loading of single H$_2^+$ molecular ions into a cryogenic linear Paul trap using (2+1) resonance-enhanced multi-photon ionization (REMPI). The H$_2^+$ ions are created by resonant two-photon excitation of H$_2$ molecules from the $X\;^1Σ_g^+$ state to the $E,F\;^1Σ_g^+$ state, followed by non-resonant one-photon ionization. The H$_2^+$ ions are produced from residual gas and sympathetically cooled by a co-trapped, laser-cooled $^9$Be$^+$ ion. By tuning the wavelength of the REMPI laser, we observe the loading of single H$_2^+$ ions via the ($ν' = 0$, $L' = 0, 1, 2, 3$) rovibrational levels of the $E,F\;^1Σ_g^+$ intermediate state. We measure the success probability for the production of H$_2^+$ in the ($ν^+ = 0$, $L^+ = 1$) state via the ($ν' = 0$, $L' = 1$) level to be 85(6)% by quantum logic spectroscopy (QLS) of the hyperfine structure of this rovibrational state. Furthermore, we load an H$_2^+$ ion via the ($ν' = 0$, $L' = 2$) level and confirm its rovibrational state to be ($ν^+ = 0$, $L^+ = 2$) by QLS. We perform QLS probes on the ion over 19 h and observe no decay of the rotationally excited state. Our work demonstrates an efficient state-selective loading mechanism for single-ion, high-precision spectroscopy of hydrogen molecular ions.

Science is founded on the benchmarking of theoretical models against experimental measurements, with the challenge that for all but the simplest systems, the calculations required for high precision become extremely challenging. $\mathrm{H}_2^+$ is the simplest stable molecule, and its structure is calculable to high precision. However, studying $\mathrm{H}_2^+$ experimentally presents significant challenges: Standard control methods such as laser cooling are not applicable due to the long lifetimes of its rotational and vibrational states. Here we solve this issue by combining buffer gas cooling to quench the $\mathrm{H}_2^+$ rovibrational excitation with quantum logic operations between $\mathrm{H}_2^+$ and a co-trapped 'helper' ion to control the molecule's hyperfine structure. This enables us to perform pure quantum state preparation, coherent control, and non-destructive readout, which we use to demonstrate high-resolution microwave spectroscopy in the hyperfine structure of $\mathrm{H}_2^+$ with a precision of 2 Hz. Our results pave the way for high precision spectroscopy of $\mathrm{H}_2^+$ in both the microwave and optical domains. Due to the wide applicability of buffer gas cooling, our method provides a general tool for molecular ion species that are hard to control with quantum logic tools alone.

While it is straightforward to count laser-cooled trapped ions by fluorescence imaging, detecting the number of dark ions embedded and sympathetically cooled in a mixed ion crystal is more challenging. We demonstrate a method to track the number of dark ions in real time with single-particle sensitivity. This is achieved by observing discrete steps in the amount of fluorescence emitted from the coolant ions while exciting secular motional resonances of dark ions. By counting the number of fluorescence steps, we can identify the number of dark ions without calibration and without relying on any physical model of the motional excitation. We demonstrate the scheme by detecting H$_2^+$ and H$_3^+$ ions embedded in a Be$^+$ ion Coulomb crystal in a linear radio frequency trap. Our method allows observing the generation and destruction of individual ions simultaneously for different types of ions. Besides high-resolution spectroscopy of dark ions, another application is the detection of chemical reactions in real time with single-particle sensitivity. This is demonstrated in this work.

We investigate the motional resonances of dual-species Coulomb crystals comprised of $^9$Be$^+$ and $^{24}$Mg$^+$ ions held in a 4-rod linear Paul trap. Our experimental data and simulations show that the secular motion of such mixed crystals has rich dynamics. Their secular spectra can differ significantly from those of pure ion crystals. We propose a simple model based on mechanical coupling with Coulomb interactions between the two different ion species that explains many features of the secular spectrum. Our findings contribute to a more reliable identification of the ion species in mixed crystals.