Christiane P. Koch

We suggest a protocol for the sympathetic cooling of a molecular asymmetric top rotor co-trapped with laser-cooled atomic ions, based on resonant coupling between the molecular ion's electric dipole moment and a common normal mode of the trapped particles. By combining sympathetic sideband laser cooling with coherent microwave excitation, we demonstrate the efficient depopulation of arbitrary rotational subspaces and the ability to cool an incoherent distribution of rotational states into a single, well-defined quantum state. This capability opens the door to exploiting the rotational Hilbert space for applications in quantum information processing and high-precision spectroscopy.

Planar rotors can be realized by confining molecular ions or charged nanoparticles together with atomic ions in a Paul trap. We study the case of molecular ions or charged nanoparticles that have an electric dipole moment which couples to modes of the common vibrational motion in the trap. We calculate the strength of the coupling with specific vibrational modes for rotor masses ranging from $10^2$ atomic units, as typical for diatomic molecules, to $10^{6}\,$ atomic units, corresponding to nanoclusters. Either, the coupling manifests as a resonant energy exchange between rotational states and one of ion crystal vibrational modes. Or, in the off-resonant case, the dipole-phonon coupling results in energy shifts. In both cases we discuss how the effect may be experimentally detected using sideband-resolved laser spectroscopy and measurements of decoherence.

Sympathetic cooling of molecular ions through the Coulomb interaction with laser-cooled atomic ions is an efficient tool to prepare translationally cold molecules without, ideally, affecting the internal state of the molecular ions. However, the electric field due to the Coulomb interaction may induce rotational transitions that change the purity of initially quantum state prepared molecules. Here, we use estimates of rotational state changes in single collisions of diatomic ions with atomic ions [arXiv:1905.02130] to determine the overall rotational excitation accumulated over the sympathetic cooling. Considering two different experimental scenarios, that of a molecular ion co-trapped with a single atomic ion and a molecular ion immersed in a Coulomb crystal of atomic ions, we also estimate the cooling time.

We demonstrate a simplified method for dissipative generation of an entangled state of two trapped-ion qubits. Our implementation produces its target state faster and with higher fidelity than previous demonstrations of dissipative entanglement generation and eliminates the need for auxiliary ions. The entangled singlet state is generated in $\sim$7 ms with a fidelity of 0.949(4). The dominant source of infidelity is photon scattering. We discuss this error source and strategies for its mitigation.

Decay of bound states due to coupling with free particle states is a general phenomenon occurring at energy scales from MeV in nuclear physics to peV in ultracold atomic gases. Such a coupling gives rise to Fano-Feshbach resonances (FFR) that have become key to understanding and controlling interactions - in ultracold atomic gases, but also between quasiparticles such as microcavity polaritons. The energy positions of FFR were shown to follow quantum chaotic statistics. In contrast, lifetimes which are the fundamental property of a decaying state, have so far escaped a similarly comprehensive understanding. Here we show that a bound state, despite being resonantly coupled to a scattering state, becomes protected from decay whenever the relative phase is a multiple of $π$. We observe this phenomenon by measuring lifetimes spanning four orders of magnitude for FFR of spin-orbit excited molecular ions with merged beam and electrostatic trap experiments. Our results provide a blueprint for identifying naturally long-lived states in a decaying quantum system.

Entanglement generation can be robust against noise in approaches that deliberately incorporate dissipation into the system dynamics. The presence of additional dissipation channels may, however, limit fidelity and speed of the process. Here we show how quantum optimal control techniques can be used to both speed up the entanglement generation and increase the fidelity in a realistic setup, whilst respecting typical experimental limitations. For the example of entangling two trapped ion qubits [Lin et al., Nature 504, 415 (2013)], we find an improved fidelity by simply optimizing the polarization of the laser beams utilized in the experiment. More significantly, an alternate combination of transitions between internal states of the ions, when combined with optimized polarization, enables faster entanglement and decreases the error by an order of magnitude.

A Ramsey-type interferometer is suggested, employing a cold trapped ion and two time-delayed off-resonant femtosecond laser pulses. The laser light couples to the molecular polarization anisotropy, inducing rotational wavepacket dynamics. An interferogram is obtained from the delay dependent populations of the final field-free rotational states. Current experimental capabilities for cooling and preparation of the initial state are found to yield an interferogram visibility of more than 80\%. The interferograms can be used to determine the polarizability anisotropy with an accuracy of about $\pm 2\%$, respectively $\pm 5\%$, provided the uncertainty in the initial populations and measurement errors are confined to within the same limits.

The electronic structure of the (LiYb)$^+$ molecular ion is investigated with two variants of the coupled cluster method restricted to single, double, and noniterative or linear triple excitations. Potential energy curves for the ground and excited states, permanent and transition electric dipole movements, and long-range interaction coefficients $C_4$ and $C_6$ are reported. The data is subsequently employed in scattering calculations and photoassociation studies. Feshbach resonances are shown to be measurable despite the ion's micromotion in the Paul trap. Molecular ions can be formed in their singlet electronic ground state by one-photon photoassociation and in triplet states by two-photon photoassociation; and control of cold atom-ion chemistry based on Feshbach resonances should be feasible. Conditions for sympathetic cooling of an Yb$^+$ ion by an ultracold gas of Li atoms are found to be favorable in the temperature range of 10$\,$mK to 10$\,$nK; and further improvements using Feshbach resonances should be possible. Overall, these results suggest excellent prospects for building a quantum simulator with ultracold Yb$^+$ ions and Li atoms.

The efficient initialization of a quantum system is a prerequisite for quantum technological applications. Here we show that several classes of quantum states of a harmonic oscillator can be efficiently prepared by means of a Jaynes-Cummings interaction with a single two-level system. This is achieved by suitably tailoring external fields which drive the dipole and/or the oscillator. The time-dependent dynamics that leads to the target state is identified by means of Optimal Control Theory (OCT) based on Krotov's method. Infidelities below $10^{-4}$ can be reached for the parameters of the experiment of the ENS group in Paris, where the oscillator is a mode of a high-Q microwave cavity and the dipole is a Rydberg transition of an atom. For this specific situation we analyze the limitations on the fidelity due to parameter fluctuations and identify robust dynamics based on pulses found using ensemble OCT. Our analysis can be extended to quantum-state preparation of continuous-variable systems in other platforms, such as trapped ions and circuit QED.