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The advancement of technologies for the precise interrogation of molecules offers exciting possibilities for new studies in the realms of precision spectroscopy and quantum technologies. Experiments in these domains often address molecular vibrations in the mid-infrared (MIR) spectral region, thus generating the need for spectrally pure and accurate MIR laser sources. Quantum-cascade lasers (QCLs) have emerged as flexible sources of coherent radiation available over a wide range of MIR frequencies. Here, we demonstrate a robust approach for the simultaneous linewidth narrowing, frequency stabilisation, and absolute frequency referencing of MIR QCLs all of which are prerequisites for precise spectroscopic experiments. Following upconversion of its radiation to the visible domain, we implement a phase lock of the QCL to a linewidth-narrowed optical frequency comb which is referenced to a remote SI-traceable primary frequency standard via a fibre link for absolute frequency calibration. To achieve a reliable frequency counting of the beat note between the QCL and the OFC, we employ redundant tracking oscillators and demonstrate a frequency instability of $5\times10^{-13}$ at 1 s and $2\times10^{-14}$ at 1000 s integration time, limited by the accuracy of our remote reference.

Quantum-logic techniques for state preparation, manipulation, and non-destructive interrogation are increasingly being adopted for experiments on single molecular ions confined in traps. The ability to control molecular ions on the quantum level via a co-trapped atomic ion offers intriguing possibilities for new experiments in the realms of precision spectroscopy, quantum information processing, cold chemistry, and quantum technologies with molecules. The present article gives an overview of the basic experimental methods, recent developments and prospects in this field.

Frequency dissemination in phase-stabilized optical fiber networks for metrological frequency comparisons and precision measurements are promising candidates to overcome the limitations imposed by satellite techniques. However, network constraints restrict the availability of dedicated channels in the commonly-used C-band. Here, we demonstrate the dissemination of an SI-traceable ultrastable optical frequency in the L-band over a 456 km fiber network with ring topology, in which telecommunication data traffic occupies the full C-band. We characterize the optical phase noise and evaluate a link instability of $4.7\cdot 10^{-16}$ at 1 s and $3.8\cdot 10^{-19}$ at 2000 s integration time, and a link accuracy of $2\cdot 10^{-18}$, which is comparable to existing metrology networks in the C-band. We demonstrate the application of the disseminated frequency by establishing the SI-traceability of a laser in a remote laboratory. Finally, we show that our metrological frequency does not interfere with data traffic in the telecommunication channels. Our approach combines an unconventional spectral choice in the telecommunication L-band with established frequency-stabilization techniques, providing a novel, cost-effective solution for ultrastable frequency-comparison and dissemination, and may contribute to a foundation of a world-wide metrological network., Comment: 10 pages, 6 figures

Quantum-logic techniques used to manipulate quantum systems are now increasingly being applied to molecules. Previous experiments on single trapped diatomic species have enabled state detection with excellent fidelities and highly precise spectroscopic measurements. However, for complex molecules with a dense energy-level structure improved methods are necessary. Here, we demonstrate an enhanced quantum protocol for molecular state detection using state-dependent forces. Our approach is based on interfering a reference and a signal force applied to a single atomic and molecular ion, respectively, in order to extract their relative phase. We use this phase information to identify states embedded in a dense molecular energy-level structure and to monitor state-to-state inelastic scattering processes. This method can also be used to exclude a large number of states in a single measurement when the initial state preparation is imperfect and information on the molecular properties is incomplete. While the present experiments focus on N$_2^+$, the method is general and is expected to be of particular benefit for polyatomic systems.

Trapped atoms and ions are among the best controlled quantum systems which find widespread applications in quantum information, sensing and metrology. For molecules, however, a similar degree of control is currently lacking owing to their complex energy-level structure. Quantum-logic protocols in which atomic ions serve as probes for molecular ions are a promising route for achieving this level of control, especially with homonuclear molecules that decouple from black-body radiation. Here, a quantum-non-demolition protocol on single trapped N$_2^+$ molecules is demonstrated. The spin-rovibronic state of the molecule is detected with more than 99% fidelity and the position and strength of a spectroscopic transition in the molecule are determined, both without destroying the molecular quantum state. The present method lays the foundations for new approaches to molecular precision spectroscopy, for state-to-state chemistry on the single-molecule level and for the implementation of molecular qubits.

We report a precise determination of the lifetime of the (4p)$^2$P$_{3/2}$ state of $^{40}$Ca$^+$, $\tau_{\textrm{P}_{3/2}}=6.639(42)$ ns, using a combination of measurements of the induced light shift and scattering rate on a single trapped ion. Good agreement with the result of a recent high-level theoretical calculation, $6.69(6)$ ns [Safronova et al., PRA 83, 012503 (2011)], but a 6-$\sigma$ discrepancy with the most precise previous experimental value, $6.924(19)$ ns [Jin et al., PRL 70, 3213 (1993)] is found. To corroborate the consistency and accuracy of the new measurements, relativistically corrected ratios of reduced-dipole-matrix elements are used to directly compare our result with a recent result for the P$_{1/2}$ state, yielding a good agreement. The application of the present method to precise determinations of radiative quantities of molecular systems is discussed.

We present theoretical and experimental progress towards a new approach for the precision spectroscopy, coherent manipulation and state-to-state chemistry of single isolated molecular ions in the gas phase. Our method consists of a molecular beam for creating packets of rotationally cold neutrals from which a single molecule is state-selectively ionized and trapped inside a radiofrequency ion trap. In addition to the molecular ion, a single co-trapped atomic ion is used to cool the molecular external degrees of freedom to the ground state of the trap and to detect the molecular state using state-selective coherent motional excitation from a modulated optical-dipole force acting on the molecule. We present a detailed discussion and theoretical characterization of the present approach. We simulate the molecular signal experimentally using a single atomic ion indicating that different rovibronic molecular states can be resolved and individually detected with our method. The present approach for the coherent control and non-destructive detection of the quantum state of a single molecular ion opens up new perspectives for precision spectroscopies relevant for, e.g., tests of fundamental physical theories and the development of new types of clocks based on molecular vibrational transitions. It will also enable the observation and control of chemical reactions of single particles on the quantum level. While focusing on N$_2^+$ as a prototypical example in the present work, our method is applicable to a wide range of diatomic and polyatomic molecules.

We demonstrate the trapping and sympathetic cooling of B$^{+}$ ions in a Coulomb crystal of laser-cooled Ca$^{+}$, We non-destructively confirm the presence of the both B$^+$ isotopes by resonant excitation of the secular motion. The B$^{+}$ ions are loaded by ablation of boron and the secular excitation spectrum also reveals features consistent with ions of the form B$_{n}^{+}$., Comment: 6 pages, 4 figures, comments welcome