Accurate Determination of Blackbody Radiation Shifts in a Strontium Molecular Lattice Clock.

Molecular lattice clocks enable the search for new physics, such as fifth forces or temporal variations of fundamental constants, in a manner complementary to atomic clocks. Blackbody radiation (BBR) is a major contributor to the systematic error budget of conventional atomic clocks and is notoriously difficult to characterize and control. Here, we combine infrared Stark-shift spectroscopy in a molecular lattice clock and modern quantum chemistry methods to characterize the polarizabilities of the Sr_{2} molecule from dc to infrared. Using this description, we determine the static and dynamic blackbody radiation shifts for all possible vibrational clock transitions to the 10^{-16} level. This constitutes an important step toward millihertz-level molecular spectroscopy in Sr_{2} and provides a framework for evaluating BBR shifts in other homonuclear molecules.

Transition Strength Measurements to Guide Magic Wavelength Selection in Optically Trapped Molecules.

Optical trapping of molecules with long coherence times is crucial for many protocols in quantum information and metrology. However, the factors that limit the lifetimes of the trapped molecules remain elusive and require improved understanding of the underlying molecular structure. Here we show that measurements of vibronic line strengths in weakly and deeply bound ^{88}Sr_{2} molecules, combined with ab initio calculations, allow for unambiguous identification of vibrational quantum numbers. This, in turn, enables the construction of refined excited potential energy curves, informing the selection of magic wavelengths that facilitate long vibrational coherence. We demonstrate Rabi oscillations between far-separated vibrational states that persist for nearly 100 ms.

Crossover from the Ultracold to the Quasiclassical Regime in State-Selected Photodissociation.

Processes that break molecular bonds are typically observed with molecules occupying a mixture of quantum states and successfully described with quasiclassical models, while a few studies have explored the distinctly quantum mechanical low-energy regime. Here, we use photodissociation of diatomic strontium molecules to demonstrate the crossover from the ultracold, quantum regime where photofragment angular distributions strongly depend on the kinetic energy to the quasiclassical regime. Using time-of-flight imaging for photodissociation channels with millikelvin reaction barriers, we explore photofragment energies in the 0.1-300 mK range experimentally and up to 3 K theoretically, and discuss the energy scale at which the crossover occurs. We find that the effects of quantum statistics can persist to high photodissociation energies.

Control of Ultracold Photodissociation with Magnetic Fields.

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 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 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.

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 (88)Sr2 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.

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.

An atom trap trace analysis system for measuring krypton contamination in xenon dark matter detectors.

We have developed an atom trap trace analysis (ATTA) system to measure Kr in Xe at the part per trillion (ppt) level, a prerequisite for the sensitivity achievable with liquid xenon dark matter detectors beyond the current generation. Since Ar and Kr have similar laser cooling wavelengths, the apparatus has been tested with Ar to avoid contamination prior to measuring Xe samples. A radio-frequency plasma discharge generates a beam of metastable atoms which is optically collimated, slowed, and trapped using standard magneto-optical techniques. Based on the measured overall system efficiency of 1.2 × 10(-8) (detection mode), we expect the ATTA system to reach the design goal sensitivity to ppt concentrations of Kr in Xe in <2 h.

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.

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.

New limits on coupling of fundamental constants to gravity using 87Sr optical lattice clocks.

The 1S0-3P0 clock transition frequency nuSr in neutral 87Sr has been measured relative to the Cs standard by three independent laboratories in Boulder, Paris, and Tokyo over the last three years. The agreement on the 1 x 10(-15) level makes nuSr the best agreed-upon optical atomic frequency. We combine periodic variations in the 87Sr clock frequency with 199Hg+ and H-maser data to test local position invariance by obtaining the strongest limits to date on gravitational-coupling coefficients for the fine-structure constant alpha, electron-proton mass ratio mu, and light quark mass. Furthermore, after 199Hg+, 171Yb+, and H, we add 87Sr as the fourth optical atomic clock species to enhance constraints on yearly drifts of alpha and mu.

Precision test of mass-ratio variations with lattice-confined ultracold molecules.

We propose a precision measurement of time variations of the proton-electron mass ratio using ultracold molecules in an optical lattice. Vibrational energy intervals are sensitive to changes of the mass ratio. In contrast to measurements that use hyperfine-interval-based atomic clocks, the scheme discussed here is model independent and does not require separation of time variations of different physical constants. The possibility of applying the zero-differential-Stark-shift optical lattice technique is explored to measure vibrational transitions at high accuracy.

Sr lattice clock at 1 x 10(-16) fractional uncertainty by remote optical evaluation with a Ca clock.

Optical atomic clocks promise timekeeping at the highest precision and accuracy, owing to their high operating frequencies. Rigorous evaluations of these clocks require direct comparisons between them. We have realized a high-performance remote comparison of optical clocks over kilometer-scale urban distances, a key step for development, dissemination, and application of these optical standards. Through this remote comparison and a proper design of lattice-confined neutral atoms for clock operation, we evaluate the uncertainty of a strontium (Sr) optical lattice clock at the 1 x 10(-16) fractional level, surpassing the current best evaluations of cesium (Cs) primary standards. We also report on the observation of density-dependent effects in the spin-polarized fermionic sample and discuss the current limiting effect of blackbody radiation-induced frequency shifts.

Narrow line photoassociation in an optical lattice.

With ultracold 88Sr in a 1D magic wavelength optical lattice, we performed narrow-line photoassociation spectroscopy near the 1S0 - 3P1 intercombination transition. Nine least-bound vibrational molecular levels associated with the long-range 0u and 1u potential energy surfaces were measured and identified. A simple theoretical model accurately describes the level positions and treats the effects of the lattice confinement on the line shapes. The measured resonance strengths show that optical tuning of the ground state scattering length should be possible without significant atom loss.

Precision measurement of the three 2(3)P(J) helium fine structure intervals.

The three 2(3)P fine structure intervals of 4H are measured at an improved accuracy that is sufficient to test two-electron QED theory and to determine the fine structure constant alpha to 14 parts in 10(9). The more accurate determination of alpha, to a precision higher than attained with the quantum Hall and Josephson effects, awaits the reconciliation of two inconsistent theoretical calculations now being compared term by term. A low pressure helium discharge presents experimental uncertainties quite different than for earlier measurements and allows direct measurements of light pressure shifts.