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1. Quantum Metrology with a Molecular Lattice Clock and State-Selected Photodissociation of Ultracold Molecules

   Lee, C.-H. (January 2020, Columbia University thesis)

   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. 

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2. Fundamental physics with a state-of-the-art optical clock in space

   https://doi.org/10.1088/2058-9565/ac7df9  

   Derevianko, Andrei; Gibble, Kurt; Hollberg, Leo; Newbury, Nathan R; Oates, Chris; Safronova, Marianna S; Sinclair, Laura C; Yu, Nan (July 2022, Quantum Science and Technology)

   Abstract Recent advances in optical atomic clocks and optical time transfer have enabled new possibilities in precision metrology for both tests of fundamental physics and timing applications. Here we describe a space mission concept that would place a state-of-the-art optical atomic clock in an eccentric orbit around Earth. A high stability laser link would connect the relative time, range, and velocity of the orbiting spacecraft to earthbound stations. The primary goal for this mission would be to test the gravitational redshift, a classical test of general relativity, with a sensitivity 30 000 times beyond current limits. Additional science objectives include other tests of relativity, enhanced searches for dark matter and drifts in fundamental constants, and establishing a high accuracy international time/geodesic reference. 

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3. Prospects of a thousand-ion Sn2+ Coulomb-crystal clock with sub-10−19 inaccuracy

   https://doi.org/10.1038/s41467-024-49241-w  

   Leibrandt, David_R; Porsev, Sergey_G; Cheung, Charles; Safronova, Marianna_S (July 2024, Nature Communications)

   Abstract Optical atomic clocks are the most accurate and precise measurement devices of any kind, enabling advances in international timekeeping, Earth science, fundamental physics, and more. However, there is a fundamental tradeoff between accuracy and precision, where higher precision is achieved by using more atoms, but this comes at the cost of larger interactions between the atoms that limit the accuracy. Here, we propose a many-ion optical atomic clock based on three-dimensional Coulomb crystals of order one thousand Sn²⁺ions confined in a linear RF Paul trap with the potential to overcome this limitation. Sn²⁺has a unique combination of features that is not available in previously considered ions: a¹S₀ ↔ ³P₀clock transition between two states with zero electronic and nuclear angular momentum (I = J = F = 0) making it immune to nonscalar perturbations, a negative differential polarizability making it possible to operate the trap in a manner such that the two dominant shifts for three-dimensional ion crystals cancel each other, and a laser-accessible transition suitable for direct laser cooling and state readout. We present calculations of the differential polarizability, other relevant atomic properties, and the motion of ions in large Coulomb crystals, in order to estimate the achievable accuracy and precision of Sn²⁺Coulomb-crystal clocks. 

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4. Multi-ensemble metrology by programming local rotations with atom movements

   https://doi.org/10.1038/s41567-023-02323-w  

   Shaw, Adam L.; Finkelstein, Ran; Tsai, Richard Bing-Shiun; Scholl, Pascal; Yoon, Tai Hyun; Choi, Joonhee; Endres, Manuel (February 2024, Nature Physics)

   Abstract Current optical atomic clocks do not utilize their resources optimally. In particular, an exponential gain in sensitivity could be achieved if multiple atomic ensembles were to be controlled or read out individually, even without entanglement. However, controlling optical transitions locally remains an outstanding challenge for neutral-atom-based clocks and quantum computing platforms. Here we show arbitrary, single-site addressing for an optical transition via sub-wavelength controlled moves of atoms trapped in tweezers. The scheme is highly robust as it relies only on the relative position changes of tweezers and requires no additional addressing beams. Using this technique, we implement single-shot, dual-quadrature readout of Ramsey interferometry using two atomic ensembles simultaneously, and show an enhancement of the usable interrogation time at a given phase-slip error probability. Finally, we program a sequence that performs local dynamical decoupling during Ramsey evolution to evolve three ensembles with variable phase sensitivities, a key ingredient of optimal clock interrogation. Our results demonstrate the potential of fully programmable quantum optical clocks even without entanglement and could be combined with metrologically useful entangled states in the future. 

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5. Multi-ensemble metrology by programming local rotations with atom movements

   Shaw, A; Finkelstein, Ran; Tsai, Richard; Scholl, Pascal; Yoon, Tai Hyun; Choi, Joonhee; Endres, Manuel (January 2024, Nature Physics)

   Current optical atomic clocks do not utilize their resources optimally. In particular, an exponential gain in sensitivity could be achieved if multiple atomic ensembles were to be controlled or read out individually, even without entanglement. However, controlling optical transitions locally remains an outstanding challenge for neutral-atom-based clocks and quantum computing platforms. Here we show arbitrary, single-site addressing for an optical transition via sub-wavelength controlled moves of atoms trapped in tweezers. The scheme is highly robust as it relies only on the relative position changes of tweezers and requires no additional addressing beams. Using this technique, we implement single-shot, dual-quadrature readout of Ramsey interferometry using two atomic ensembles simultaneously, and show an enhancement of the usable interrogation time at a given phase-slip error probability. Finally, we program a sequence that performs local dynamical decoupling during Ramsey evolution to evolve three ensembles with variable phase sensitivities, a key ingredient of optimal clock interrogation. Our results demonstrate the potential of fully programmable quantum optical clocks even without entanglement and could be combined with metrologically useful entangled states in the future. 

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