Abstract With relative accuracies reaching 10−18, optical atomic clocks are currently the most sensitive physical instruments known to man. Weakly bound ultracold molecules enable the study of fundamental physics through their sensitivity to e.g. the proton-to-electron mass ratio or hypothetical Yukawa-type fifth forces predicted by several extensions of the Standard Model. These applications, however, require precision measurements of molecular transitions that are beyond current experimental capabilities. Here we propose to construct an ‘optical molecular clock’ that would solve this problem by bringing the experimental techniques used in optical atomic clocks to the realm of cold molecules. We show that such a clock could utilize ultracold ytterbium molecules and we predict the positions and properties of Yb2 clock lines. A successful experimental realization of this proposal could pave the way towards sub-Hz level molecular spectroscopy.
Abstract With relative accuracies reaching 10−18, optical atomic clocks are currently the most sensitive physical instruments known to man. Weakly bound ultracold molecules enable the study of fundamental physics through their sensitivity to e.g. the proton-to-electron mass ratio or hypothetical Yukawa-type fifth forces predicted by several extensions of the Standard Model. These applications, however, require precision measurements of molecular transitions that are beyond current experimental capabilities. Here we propose to construct an ‘optical molecular clock’ that would solve this problem by bringing the experimental techniques used in optical atomic clocks to the realm of cold molecules. We show that such a clock could utilize ultracold ytterbium molecules and we predict the positions and properties of Yb2 clock lines. A successful experimental realization of this proposal could pave the way towards sub-Hz level molecular spectroscopy.
Optical molecular clocks promise unparalleled sensitivity to the temporal variation of the electron-to-proton mass ratio and insight into possible new physics beyond the standard model. We propose to realize a molecular clock with bosonic ^{174}Yb_{2} molecules, where the forbidden ^{1}S_{0}→^{3}P_{0} clock transition would be induced magnetically. The use of a bosonic species avoids possible complications due to the hyperfine structure present in fermionic species. While direct clock line photoassociation would be challenging, weakly bound ground state molecules could be produced by stimulated Raman adiabatic passage and used instead. The recent scattering measurements [L. Franchi, et al. New J. Phys. 19, 103037 (2017)NJOPFM1367-263010.1088/1367-2630/aa8fb4] enable us to determine the positions of target ^{1}S_{0}+^{3}P_{0} vibrational levels and calculate the Franck-Condon factors for clock transitions between ground and excited molecular states. The resulting magnetically induced Rabi frequencies are similar to those for atoms hinting that an experimental realization is feasible. A successful observation could pave the way towards Hz-level molecular spectroscopy.
Abstract : We have established the strontium molecular clock as the leading ultracold-molecule precision measurement platform. We can fully control the molecules internal and external quantum states, as in state-of-the-art atomic lattice clocks. Using the quantized molecular spectra in an optical lattice, we devised a new lattice thermometry method that is advantageous for many lattice experiments, including clocks and manybody physics studies. The full quantum control allowed us to observe deeply subradiant molecular states, and coherently control them. We measured lifetimes enhanced by up to 300 times. Ultranarrow transitions to these states permitted a rigorous study of asymptotic physics at the atom-molecule threshold. We proved that subradiant states can decay to the ground state via higher-order electromagnetic transitions, with a rate that grows as the square of the bond length, and are quenched by predissociation at a rate proportional to the vibrational level spacing. We introduced a precise technique for measuring molecular binding energies via photofragmentation; controlled forbidden optical transition strengths with weak magnetic fields by five orders of magnitude; and explained anomalously large magnetic susceptibilities of the asymptotic molecules. The unprecedented precision, coupled with advanced ab initio theory, paves the way to exciting new directions for the molecular clock.
Ultracold molecules are a powerful platform for metrology, precision measurements and searches for new, beyond-the-Standard-Model physics. Sr2, thanks to its simple structure, insensitivity to external fields and narrow optical transitions, provides an excellent testbed for the search for new interactions. Here, we present a detailed characterization of our 88Sr2 molecular clock for a vibrational transition spanning the entire depth of the ground state potential. We also discuss prospects to use strontium isotopologues to place improved constraints on new mass-dependent forces, including possible pathways toward the production of ultracold 86Sr2 and 84Sr2 dimers and spectroscopy of clock lines in these species for use in the search for new mass-dependent forces.
Over the past few decades, rapid development of laser cooling techniques and narrow-linewidth lasers have allowed atom-based quantum clocks to achieve unprecedented precision. Techniques originally developed for atomic clocks can be extended to ultracold molecules, with applications ranging from quantum-state-controlled ultracold chemistry to searches for new physics. Because of the richness of molecular structure, quantum metrology based on molecules provides possibilities for testing physics that is beyond the scope of traditional atomic clocks. This thesis presents the work performed to establish a state-of-the-art quantum clock based on ultracold molecules. The molecular clock is based on a frequency difference between two vibrational levels in the electronic ground state of 88Sr2 diatomic molecules. Such a clock allows us test molecular QED, improve constraints on nanometer-scale gravity, and potentially provide a model-independent test of temporal variations of the proton-electron mass ratio. Trap-insensitive spectroscopy is crucial for extending coherent molecule-light interactions and achieving a high quality factor Q. We have demonstrated a magic wavelength technique for molecules by manipulating the optical lattice frequency near narrow polarizability resonances. This general technique allows us to increase the coherence time to tens of ms, an improvement of a factor of several thousand, and to narrow the linewidth of a 25 THz vibrational transition initially to 30 Hz. This width corresponds to the quality factor Q=8x10^11. Besides the molecular quantum metrology, investigations of novel phenomena in state-selected photodissociation are also described in this thesis, including magnetic-field control of photodissociation and observation of the crossover from ultracold to quasiclassical chemistry.
Cooling and trapping of neutral atoms using laser techniques has enabled extensive progress in precise, coherent spectroscopy. In particular, trapping ultracold atoms in optical lattices in a tight confinement regime allows us to perform high-resolution spectroscopy unaffected by atomic motion. We report on the recent developments of optical lattice atomic clocks that have led to optical spectroscopy coherent at the one second timescale. The lattice clock techniques also open a promising pathway toward trapped ultracold molecules and the possible precision measurement opportunities such molecules offer.
An optical lattice clock probes a spectrally narrow electronic transition in an ensemble of optically trapped, laser-cooled atoms, for use as a time and frequency standard. To date, several lattice clocks have been demonstrated with superior stability and accuracy compared to primary frequency standards based on microwave transitions. Yet, the question of which atomic system (including the element and isotope) performs best as a lattice clock remains unsettled. This thesis describes the first detailed investigation of an optical lattice clock using a spin-1/2 isotope of the ytterbium atom. A spin-1/2 system possesses several advantages over higher-spin systems, including a simplified level structure (allowing for straightforward manipulation of the nuclear spin state) and the absence of any tensor light shift from the confining optical lattice. Moreover, the ytterbium atom (Yb) stands among the leading lattice clock candidates, offering a high-performance optical clock with some degree of experimental simplicity. The frequency stability of the Yb clock is highlighted by resolving an ultra-narrow clock spectrum with a full-width at half-maximum of 1 Hz, corresponding to a record quality factor Q = ν0/Δν = 5 × 1014. Moreover, this system can be highly accurate, which is demonstrated by characterizing the Yb clock frequency at the 3 × 10-16 level of fractional uncertainty, with further progress toward a ten-fold improvement also presented. To reach this low level of uncertainty required careful consideration of important systematic errors, including the identification of the Stark-canceling wavelength, where the clock’s sensitivity to the lattice intensity is minimized, a precise determination of the static polarizability of the clock transition, and the measurement and control of atom-atom collisions.