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arXiv:1802.08291 · Physical Review Letters

Optical Lattice Clocks with Weakly Bound Molecules

Mateusz Borkowski

Published Feb 22, 2018• 28 citations
arXivHTMLPDF

Abstract

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.

DOI
10.1103/physrevlett.120.083202

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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 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.
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.
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.
We observe a weakly allowed optical transition of atomic ytterbium from the ground state to the metastable state 4f^{13}5d6s^{2} (J=2) for all five bosonic and two fermionic isotopes with resolved Zeeman and hyperfine structures. This inner-shell orbital transition has been proposed as a new frequency standard as well as a quantum sensor for new physics. We find magic wavelengths through the measurement of the scalar and tensor polarizabilities and reveal that the measured trap lifetime in a three-dimensional optical lattice is 1.9(1) s, which is crucial for precision measurements. We also determine the g factor by an interleaved measurement, consistent with our relativistic atomic calculation. This work opens the possibility of an optical lattice clock with improved stability and accuracy as well as novel approaches for physics beyond the standard model.
Ultracold paramagnetic and polar diatomic molecules are among the promising systems for quantum simulation of lattice-spin models. Unfortunately, their experimental observation is still challenging. Based on our recent ab initio calculations, we analyze the feasibility of all-optical schemes for the formation of ultracold 87Rb84Sr^{87}\mathrm{Rb}^{84}\mathrm{Sr}87Rb84Sr bosonic molecules. A first possibility is photoassociation followed by spontaneous emission. The photoassociation rate coefficients toward electronic states converging to the 87Rb(5s2S1/2)+84Sr(5s5p3P0,1,2^{87}\mathrm{Rb}(5s\phantom{\rule{0.16em}{0ex}}^{2}S_{1/2})+^{84}\mathrm{Sr}(5s5p\phantom{\rule{0.16em}{0ex}}^{3}P_{0,1,2}87Rb(5s2S1/2​)+84Sr(5s5p3P0,1,2​) asymptotes are particularly small for vibrational levels close to the asymptote. The creation of molecules would be more interesting by using deeply bound levels which preferentially relax to the ${v}^{\ensuremath{'}\ensuremath{'}}=0$ level of the ground state. On the other hand, the photoassociation rate coefficients toward electronic states correlated to the Rb(5p2P1/2,3/2)+Sr(5s21S0\mathrm{Rb}(5p\phantom{\rule{0.16em}{0ex}}^{2}P_{1/2,3/2})+\mathrm{Sr}(5{s}^{2}\phantom{\rule{0.16em}{0ex}}^{1}S_{0}Rb(5p2P1/2,3/2​)+Sr(5s21S0​) are significant for levels close to the asymptote. The spontaneous emission thus creates weakly bound molecules in a single vibrational level. A second option relies on stimulated Raman adiabatic passage implemented in a tight optical trap. It efficiently creates weakly bound ground-state molecules in a well-defined level, thus providing a promising alternative to magnetic Feshbach resonances for further population transfer toward the absolute ground state of the RbSr molecule.
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.