Chunyan Shi

Precision spectroscopy has been the driving force for progress of our physical understanding and still is a promising tool for the investigation of new physics. Molecules offer transitions which allow tests that are not possible in atomic systems. However, usually precision spectroscopy of molecules is challenging due to the lack of cycling transitions for state preparation and state detection. For molecular ions, this obstacle can be overcome by quantum logic spectroscopy, where dissipation for state preparation and detection is provided by a co-trapped atomic ion exploiting the shared eigenstates of motion. Here, we propose a full quantum logic spectroscopy scheme for molecular oxygen ions and theoretically investigate the feasibility of quantum logic assisted state detection and preparation. Furthermore, we provide coupling rates for a direct single-photon quadrupole excitation of a vibrational overtone transition that can serve as a sensitive transition for tests of a possible variation of the proton-to-electron mass ratio.

Non-vanishing fluctuations of the vacuum state are a salient feature of quantum theory. These fluctuations fundamentally limit the precision of quantum sensors. Nowadays, several systems such as optical clocks, gravitational wave detectors, matter-wave interferometers, magnetometers, and optomechanical systems approach measurement sensitivities where the effect of quantum fluctuations sets a fundamental limit, the so-called standard quantum limit (SQL). It has been proposed that the SQL can be overcome by squeezing the vacuum fluctuations. Realizations of this scheme have been demonstrated in various systems. However, protocols based on squeezed vacuum crucially rely on precise control of the relative orientation of the squeezing with respect to the operation imprinting the measured quantity. Lack of control can lead to an amplification of noise and reduces the sensitivity of the device. Here, we experimentally demonstrate a novel quantum metrological paradigm based on phase insensitive Fock states of the motional state of a trapped ion, with applications in frequency metrology and displacement detection. The measurement apparatus is used in two different experimental settings probing non-commuting observables with sensitivities beyond the SQL. In both measurements, classical preparation and detection noise are sufficiently small to preserve the quantum gain in a full metrological protocol.

Laser spectroscopy of cold and trapped molecular ions is a powerful tool for fundamental physics, including the determination of fundamental constants, the laboratory test for their possible variation, and the search for a possible electric dipole moment of the electron. Optical clocks based on molecular ions sensitive to some of these effects are expected to achieve uncertainties approaching the $10^{-18}$ level. While the complexity of molecular structure facilitates these applications, the absence of cycling transitions poses a challenge for direct laser cooling, quantum state control, and detection. Previously employed state detection techniques based on photo-dissociation or chemical reactions are destructive and therefore inefficient. Here we experimentally demonstrate non-destructive state detection of a single trapped molecular ion through its strong Coulomb coupling to a well-controlled co-trapped atomic ion. An algorithm based on a state-dependent optical dipole force(ODF) changes the internal state of the atom conditioned on the internal state of the molecule. We show that individual states in the molecule can be distinguished by their coupling strength to the ODF and observe black-body radiation-induced quantum jumps between rotational states. Using the detuning dependence of the state detection signal, we implement a variant of quantum logic spectroscopy and improve upon a previous measurement of the $\mathrm{X}^1Σ^+(J=1)\rightarrow\mathrm{A}^1Σ^+(J=0)$ transition in MgH, finding a frequency of 1067.74752(53)THz. We estimate that non-destructive state detection with near 100% efficiency could take less than 10 ms. The technique we demonstrate is applicable to a wide range of molecular ions, enabling further applications in state-controlled quantum chemistry and spectroscopic investigations of molecules serving as probes for interstellar clouds.