No Arabic abstract
In weakly bound diatomic molecules, energy levels are closely spaced and thus more susceptible to mixing by magnetic fields than in the constituent atoms. We use this effect to control the strengths of forbidden optical transitions in $^{88}$Sr$_2$ over 5 orders of magnitude with modest fields by taking advantage of the intercombination-line threshold. The physics behind this remarkable tunability is accurately explained with both a simple model and quantum chemistry calculations, and suggests new possibilities for molecular clocks. We show how mixed quantization in an optical lattice can simplify molecular spectroscopy. Furthermore, our observation of formerly inaccessible $f$-parity excited states offers an avenue for improving theoretical models of divalent-atom dimers.
We observe trilobite-like states of ultracold 85Rb2 molecules, in which a ground-state atom is bound by the electronic wavefunction of its Rydberg-atom partner. We populate these states through the ultraviolet excitation of weakly-bound molecules, and access a regime of trilobite-like states at low principal quantum numbers and with vibrational turning points around 35 Bohr radii. This demonstrates that, unlike previous studies that used free-to-bound transitions, trilobite-like states can also be excited through bound-to-bound transitions. This approach provides high excitation probabilities without requiring high-density samples, and affords the ability to control the excitation radius by selection of the initial-state vibrational level.
Photodissociation of a molecule produces a spatial distribution of photofragments determined by the molecular structure and the characteristics of the dissociating light. Performing this basic chemical reaction at ultracold temperatures allows its quantum mechanical features to dominate. In this regime, weak applied fields can be used to control the reaction. Here, we photodissociate ultracold diatomic strontium in magnetic fields below 10 G and observe striking changes in photofragment angular distributions. The observations are in excellent qualitative agreement with a multichannel quantum chemistry model that includes nonadiabatic effects and predicts strong mixing of partial waves in the photofragment energy continuum. The experiment is enabled by precise quantum-state control of the molecules.
Chemical reactions at ultracold temperatures are expected to be dominated by quantum mechanical effects. Although progress towards ultracold chemistry has been made through atomic photoassociation, Feshbach resonances and bimolecular collisions, these approaches have been limited by imperfect quantum state selectivity. In particular, attaining complete control of the ground or excited continuum quantum states has remained a challenge. Here we achieve this control using photodissociation, an approach that encodes a wealth of information in the angular distribution of outgoing fragments. By photodissociating ultracold 88Sr2 molecules with full control of the low-energy continuum, we access the quantum regime of ultracold chemistry, observing resonant and nonresonant barrier tunneling, matter-wave interference of reaction products and forbidden reaction pathways. Our results illustrate the failure of the traditional quasiclassical model of photodissociation and instead are accurately described by a quantum mechanical model. The experimental ability to produce well-defined quantum continuum states at low energies will enable high-precision studies of long-range molecular potentials for which accurate quantum chemistry models are unavailable, and may serve as a source of entangled states and coherent matter waves for a wide range of experiments in quantum optics.
Qubit coherence times are critical to the performance of any robust quantum computing platform. For quantum information processing using arrays of polar molecules, a key performance parameter is the molecular rotational coherence time. We report a 93(7) ms coherence time for rotational state qubits of laser cooled CaF molecules in optical tweezer traps, over an order of magnitude longer than previous systems. Inhomogeneous broadening due to the differential polarizability between the qubit states is suppressed by tuning the tweezer polarization and applied magnetic field to a magic angle. The coherence time is limited by the residual differential polarizability, implying improvement with further cooling. A single spin-echo pulse is able to extend the coherence time to nearly half a second. The measured coherence times demonstrate the potential of polar molecules as high fidelity qubits.
We present a novel method for engineering an optical clock transition that is robust against external field fluctuations and is able to overcome limits resulting from field inhomogeneities. The technique is based on the application of continuous driving fields to form a pair of dressed states essentially free of all relevant shifts. Specifically, the clock transition is robust to magnetic shifts, quadrupole and other tensor shifts, and amplitude fluctuations of the driving fields. The scheme is applicable to either a single ion or an ensemble of ions, and is relevant for several types of ions, such as $^{40}mathrm{Ca}^{+}$, $^{88}mathrm{Sr}^{+}$, $^{138}mathrm{Ba}^{+}$ and $^{176}mathrm{Lu}^{+}$. Taking a spherically symmetric Coulomb crystal formed by 400 $^{40}mathrm{Ca}^{+}$ ions as an example, we show through numerical simulations that the inhomogeneous linewidth of tens of Hertz in such a crystal together with linear Zeeman shifts of order 10~MHz are reduced to form a linewidth of around 1~Hz. We estimate a two-order-of-magnitude reduction in averaging time compared to state-of-the art single ion frequency references, assuming a probe laser fractional instability of $10^{-15}$. Furthermore, a statistical uncertainty reaching $2.9times 10^{-16}$ in 1~s is estimated for a cascaded clock scheme in which the dynamically decoupled Coulomb crystal clock stabilizes the interrogation laser for an $^{27}mathrm{Al}^{+}$ clock.