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1. An optical tweezer array of ultracold polyatomic molecules

   https://doi.org/10.1038/s41586-024-07199-1  

   Vilas, Nathaniel B; Robichaud, Paige; Hallas, Christian; Li, Grace K; Anderegg, Loïc; Doyle, John M (April 2024, Nature)

   Polyatomic molecules have rich structural features that make them uniquely suited to applications in quantum information science1–3, quantum simulation4–6, ultracold chemistry7 and searches for physics beyond the standard model8–10. However, a key challenge is fully controlling both the internal quantum state and the motional degrees of freedom of the molecules. Here we demonstrate the creation of an optical tweezer array of individual polyatomic molecules, CaOH, with quantum control of their internal quantum state. The complex quantum structure of CaOH results in a non-trivial dependence of the molecules’ behaviour on the tweezer light wavelength. We control this interaction and directly and non-destructively image individual molecules in the tweezer array with a fidelity greater than 90%. The molecules are manipulated at the single internal quantum state level, thus demonstrating coherent state control in a tweezer array. The platform demonstrated here will enable a variety of experiments using individual polyatomic molecules with arbitrary spatial arrangement. 

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2. Raman sideband cooling of molecules in an optical tweezer array

   https://doi.org/10.1038/s41567-023-02346-3  

   Lu, Yukai; Li, Samuel J.; Holland, Connor M.; Cheuk, Lawrence W. (March 2024, Nature Physics)

   Ultracold molecules have been proposed as a candidate platform for quantum science and precision measurement because of their rich internal structures and interactions. Direct laser-cooling promises to be a rapid and efficient way to bring molecules to ultracold temperatures. However, for trapped molecules, laser-cooling to the quantum motional ground state remains an outstanding challenge. A technique capable of reaching the motional ground state is Raman sideband cooling, first demonstrated in trapped ions and atoms. Here we demonstrate Raman sideband cooling of CaF molecules trapped in an optical tweezer array. Our protocol does not rely on high magnetic fields and preserves the purity of molecular internal states. We measure a high ground-state fraction and achieve low motional entropy per particle. The low temperatures we obtain could enable longer coherence times and higher-fidelity molecular qubit gates, desirable for quantum information processing and quantum simulation. With further improvements, Raman sideband cooling will also provide a route to quantum degeneracy of large molecular samples, which could be extendable to polyatomic molecular species. 

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3. Direct laser cooling of a symmetric top molecule

   https://doi.org/10.1126/science.abc5357  

   Mitra, Debayan; Vilas, Nathaniel B.; Hallas, Christian; Anderegg, Loïc; Augenbraun, Benjamin L.; Baum, Louis; Miller, Calder; Raval, Shivam; Doyle, John M. (September 2020, Science)

   Ultracold polyatomic molecules have potentially wide-ranging applications in quantum simulation and computation, particle physics, and quantum chemistry. For atoms and small molecules, direct laser cooling has proven to be a powerful tool for quantum science in the ultracold regime. However, the feasibility of laser-cooling larger, nonlinear polyatomic molecules has remained unknown because of their complex structure. We laser-cooled the symmetric top molecule calcium monomethoxide (CaOCH₃), reducing the temperature of ~10⁴molecules from 22 ± 1 millikelvin to 1.8 ± 0.7 millikelvin in one dimension and state-selectively cooling two nuclear spin isomers. These results demonstrate that the use of proper ro-vibronic transitions enables laser cooling of nonlinear molecules, thereby opening a path to efficient cooling of chiral molecules and, eventually, optical tweezer arrays of complex polyatomic species. 

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4. 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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5. Rotational magic conditions for ultracold molecules in the presence of Raman and Rayleigh scattering

   https://doi.org/10.1088/1367-2630/ad56bf  

   Kotochigova, Svetlana; Guan, Qingze; Tiesinga, Eite; Scarola, Vito; DeMarco, Brian; Gadway, Bryce (June 2024, New Journal of Physics)

   Abstract Molecules have vibrational, rotational, spin-orbit and hyperfine degrees of freedom or quantum states, each of which responds in a unique fashion to external electromagnetic radiation. The control over superpositions of these quantum states is key to coherent manipulation of molecules. For example, the better the coherence time the longer quantum simulations can last. The important quantity for controlling an ultracold molecule with laser light is its complex-valued molecular dynamic polarizability. Its real part determines the tweezer or trapping potential as felt by the molecule, while its imaginary part limits the coherence time. Here, our study shows that efficient trapping of a molecule in its vibrational ground state can be achieved by selecting a laser frequency with a detuning on the order of tens of GHz relative to an electric-dipole-forbidden molecular transition. Close proximity to this nearly forbidden transition allows to create a sufficiently deep trapping potential for multiple rotational states without sacrificing coherence times among these states from Raman and Rayleigh scattering. In fact, we demonstrate that magic trapping conditions for multiple rotational states of the ultracold²³Na⁸⁷Rb polar molecule can be created. 

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