Extending quantum control to increasingly complex systems is crucial for both advancing quantum technologies and fundamental physics. In trapped ion systems, quantum logic techniques that combine a well-controlled logic species with a more complex spectroscopy species have proven to be a powerful tool for extending the range of accessible species. Here, we demonstrate that a quantum system as complex as ^{48}Ti^{+} with its many metastable states can be controlled employing a combination of intrinsic thermalization due to collisions with background gas and quantum-logic techniques using a far-detuned Raman laser. The preparation of pure quantum states allows coherent manipulation and high resolution measurements of the Zeeman structure in ^{48}Ti^{+}. The presented techniques are applicable to a wide range of ionic species giving access to a larger variety of systems for fundamental physics and constitute the first step for quantum-controlled spectroscopy of transition metals, relevant, e.g., for the interpretation of astrophysical spectra.
Extending quantum control to increasingly complex systems is crucial for both advancing quantum technologies and fundamental physics. In trapped ion systems, quantum logic techniques that combine a well-controlled logic species with a more complex spectroscopy species have proven to be a powerful tool for extending the range of accessible species. Here, we demonstrate that a quantum system as complex as ^{48}Ti^{+} with its many metastable states can be controlled employing a combination of intrinsic thermalization due to collisions with background gas and quantum-logic techniques using a far-detuned Raman laser. The preparation of pure quantum states allows coherent manipulation and high resolution measurements of the Zeeman structure in ^{48}Ti^{+}. The presented techniques are applicable to a wide range of ionic species giving access to a larger variety of systems for fundamental physics and constitute the first step for quantum-controlled spectroscopy of transition metals, relevant, e.g., for the interpretation of astrophysical spectra.
High-precision spectroscopy of atomic and molecular ions is an established platform for investigating fundamental aspects of physics. An important step in this direction was the development of quantum logic techniques that enable the spectroscopy of ions whose electronic structure does not allow direct laser cooling. Particularly challenging in this context is the investigation of atomic and molecular systems with many long-lived metastable states. The preparation of a pure quantum state for spectroscopy purposes often requires the prior detection of these long-lived states. For molecular ions, schemes for the detection of their rotational degree of freedom have already been developed in the past. However, quantum logic control of transition metals, in which the many metastable states result from several valence electrons, remained elusive. In this cumulative thesis, the first experimental implementation of a quantum logic assisted scheme for internal state detection of atomic systems as complex as a titanium ion is presented. Furthermore, a scheme based on simultaneous co-magnetometry for measuring the Landé g factor was developed and demonstrated for different fine structure states in 48Ti+. The presented method allows the suppression of systematic uncertainties arising from varying magnetic fields at the position of the ion and can be transferred to a variety of other species. Crucial for quantum logic based applications is the reliable preparation of a two-ion crystal consisting of one spectroscopy ion and one logic ion. A third aspect of this work is the deterministic preparation of such a two-ion crystal. The method based on fluorescence imaging is associated with a significantly reduced calibration effort compared to other schemes and can be easily transferred to other combinations of spectroscopy and logic ions. The quantum logic control capabilities demonstrated in this work are applicable to a wide range of other atoms with complex electronic structures as well as to molecular ions. The investigation of transition metals can provide important reference data for the calibration of absorption spectra from astrophysical objects. Molecular ions have applications in the search for a possible variation of fundamental constants or the measurement of energy shifts caused by an electron electric dipole moment, both representing promising approaches to test the standard model of particle physics.
Quantum logic enables state preparation, readout and spectroscopy of otherwise difficult-to-study ions. Using the coupled harmonic motion shared between co-trapped ions, information can be transferred from the "spectroscopy" ion to the easily manipulated "logic" ion. With this technique we perform high-resolution terahertz-scale rotational spectroscopy of a single CaH+ molecular ion in pure states by leveraging a Ca+ ion as our logic ion. Entangled states between a CaH+ and a Ca+ have also been demonstrated, making molecular ions possible components of hybrid systems for quantum information processing. Because all our laser operations on the molecule are driving stimulated Raman transitions with high detuning, the technique promises to be generalizable to a wide variety of molecular ion species. Additionally, we study the systematic effects of the trap RF electric field on molecular levels and use it to obtain a measurement of the dipole moment of the charged molecule.
Preparing molecules at rest and in a very pure quantum state is a long-standing aspiration in chemistry and physics, so far achieved only for a select set of molecules in dedicated experimental setups. Here, a quantum-limited combination of mass spectrometry and Raman spectroscopy is proposed that should be applicable to a wide range of molecular ions. Excitation of electrons in the molecule followed by uncontrolled decay and branching into several lower-energy states is avoided. Instead, the molecule is always confined to rotational states within the electronic and vibrational ground-state manifold, while a co-trapped atomic ion provides efficient entropy removal and allows for extraction of information about the molecule. The outlined techniques might enable the preparation, manipulation and measurement of a multitude of molecular ion species with the same instrument, with applications including, but not limited to, precise determination of molecular properties and fundamental tests of physics.
Abstract. Preparing molecules at rest and in a highly pure quantum state is a long standing dream in chemistry and physics, so far achieved only for a select set of molecules in dedicated experimental setups. Here, a quantum-limited combination of mass spectrometry and Raman spectroscopy is proposed that should be applicable to a wide range of molecular ions. Excitation of electrons in the molecule followed by uncontrolled decay and branching into several lower energy states is avoided. Instead, the molecule is always confined to rotational states within the electronic and vibrational ground-state manifold, while a co-trapped atomic ion provides efficient entropy removal and allows for extraction of information on the molecule. The outlined techniques might enable preparation, manipulation and measurement of a large multitude of molecular ion species with the same instrument, with applications including, but not limited to, precise determination of molecular properties and fundamental tests of physics. 1.
In quantum logic spectroscopy (QLS), one species of trapped ion is used as a sensor to detect the state of an otherwise inaccessible ion species. This extends precision measurements to a broader class of atomic and molecular systems for applications like atomic clocks and tests of fundamental physics. Here, we develop a new technique based on a Schrödinger cat interferometer to address the problem of scaling QLS to larger ion numbers. We demonstrate the basic features of this method using various combinations of ^{25}Mg^{+} logic ions and ^{27}Al^{+} spectroscopy ions. We observe higher detection efficiency by increasing the number of ^{25}Mg^{+} ions. Applied to multiple ^{27}Al^{+}, this method will improve the stability of high-accuracy optical clocks and could enable Heisenberg-limited QLS.
Scaling trapped-ion quantum sensors from single ions to large ensembles is a key challenge for next-generation precision measurements. At the same time, many ion species of interest for optical clocks and tests of fundamental physics lack closed cycling transitions required for direct laser cooling and state detection. Collective quantum logic spectroscopy addresses both limitations by coupling an ensemble of sensor, or spectroscopy, ions to one or more logic ions that provide sympathetic cooling and state readout. Here, we establish the fundamental performance limits and operating regimes of this protocol, identifying how the interaction strength, interrogation time, and logic-ensemble size govern sensitivity, dynamic range, and robustness to experimental imperfections. We show that quantum-limited sensitivity can be retained even with a single logic ion, while increasing the number of logic ions substantially improves readout efficiency and robustness. Beyond precision metrology, the same collective interface enables many-body measurements relevant to quantum information processing, including parity measurements and stabilizer-like syndrome extraction. Our results establish collective quantum logic spectroscopy as a scalable framework for optical clocks, quantum-enhanced sensing, and trapped-ion quantum information processing.