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Precision measurements with ultracold atoms and molecules are primed to probe beyond-the-standard model physics. Isotopologues of homonuclear molecules are a natural testbed for new Yukawa-type mass-dependent forces at nanometer scales, complementing existing mesoscopic-body and neutron scattering experiments. Here, we propose using isotopic shift measurements in molecular lattice clocks to constrain these new interactions from new massive scalar particles in the $\mathrm{keV}/c^2$range: The new interaction would impart an extra isotopic shift to molecular levels on top of one predicted by the standard model. For the strontium dimer, a Hz-level agreement between experiment and theory could constrain the coupling of the new particles to hadrons by up to an order of magnitude over the most stringent existing experiments. Published by the American Physical Society2024 

Quantum sensing and metrology use coherent superposition states of quantum systems to detect and measure physical effects of interest. Their sensitivity is typically limited by the standard quantum limit, which bounds the achievable precision in measurements involving nominally identical but uncorrelated quantum systems. Fully quantum metrology involves entanglement in an array of quantum systems, enabling uncertainty reduction below the standard quantum limit. Although ultracold atoms have been widely used for applications such as atomic clocks or gravitational sensors, molecules show higher sensitivity to many interesting phenomena, including the existence of new, symmetry-violating forces mediated by massive particles. Recent advancements in molecular cooling, trapping and control techniques have enabled the use of molecules for quantum sensing and metrology. This Review describes these advancements and explores the potential of the rich internal structure and enhanced coupling strengths of molecules to probe fundamental physics and drive progress in the field. 

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 = 8 × 10^11. 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.