Mickey McDonald

Precise study of asymptotic physics with subradiant ultracold molecules

An experimental study characterizes subradiance—inhibited emission due to destructive interference—in ultracold molecules close to the dissociation limit and shows that it could be used for precision molecular spectroscopy. Weakly bound molecules have physical properties without atomic analogues, even as the bond length approaches dissociation. For instance, the internal symmetries of homonuclear diatomic molecules result in the formation of two-body superradiant and subradiant excited states. Whereas superradiance1,2,3 has been demonstrated in a variety of systems, subradiance4,5,6 is more elusive owing to the inherently weak interaction with the environment. Here we characterize the properties of deeply subradiant molecular states with intrinsic quality factors exceeding 1013 via precise optical spectroscopy with the longest molecule–light coherent interaction times to date. We find that two competing effects limit the lifetimes of the subradiant molecules, with different asymptotic behaviours. The first is radiative decay via weak magnetic-dipole and electric-quadrupole interactions. We prove that its rate increases quadratically with the bond length, confirming quantum mechanical predictions. The second is non-radiative decay through weak gyroscopic predissociation, with a rate proportional to the vibrational mode spacing and sensitive to short-range physics. This work bridges the gap between atomic and molecular metrology based on lattice-clock techniques7, enhancing our understanding of long-range interatomic interactions.

Optical production of stable ultracold (88)Sr(2) molecules.

We have produced large samples of stable ultracold (88)Sr(2) molecules in the electronic ground state in an optical lattice. The fast, all-optical method of molecule creation involves a near-intercombination-line photoassociation pulse followed by spontaneous emission with a near-unity Franck-Condon factor. The detection uses excitation to a weakly bound electronically excited vibrational level corresponding to a very large dimer and yields a high-Q molecular vibronic resonance. This is the first of two steps needed to create deeply bound (88)Sr(2) for frequency metrology and ultracold chemistry.

Nonadiabatic Effects in Ultracold Molecules via Anomalous Linear and Quadratic Zeeman Shifts

Anomalously large linear and quadratic Zeeman shifts are measured for weakly bound ultracold 88Sr2 molecules near the intercombination-line asymptote. Nonadiabatic Coriolis coupling and the nature of long-range molecular potentials explain how this effect arises and scales roughly cubically with the size of the molecule. The linear shifts yield nonadiabatic mixing angles of the molecular states. The quadratic shifts are sensitive to nearby opposite f-parity states and exhibit fourth-order corrections, providing a stringent test of a state-of-the-art ab initio model.

Thermometry via Light Shifts in Optical Lattices

For atoms or molecules in optical lattices, conventional thermometry methods are often unsuitable due to low particle numbers or a lack of cycling transitions. However, a differential spectroscopic light shift can map temperature onto the line shape with a low sensitivity to trap anharmonicity. We study narrow molecular transitions to demonstrate precise frequency-based lattice thermometry, as well as carrier cooling. This approach should be applicable down to nanokelvin temperatures. We also discuss how the thermal light shift can affect the accuracy of optical lattice clocks.

Photodissociation of ultracold diatomic strontium molecules with quantum state control.

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 tunnelling, 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.

Control of Optical Transitions with Magnetic Fields in Weakly Bound Molecules.

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)Sr2 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.

High-precision spectroscopy of ultracold molecules in an optical lattice

The study of ultracold molecules tightly trapped in an optical lattice can expand the frontier of precision measurement and spectroscopy, and provide a deeper insight into molecular and fundamental physics. Here we create, probe, and image microkelvin

Feedback and harmonic locking of slot-type optomechanical oscillators to external low-noise reference clocks

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Extended ultrahigh-Q-cavity diode laser

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Visible optical beats at the hertz level

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