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Long-range and anisotropic dipolar interactions profoundly modify the dynamics of particles hopping in a periodic lattice potential. We report the realization of a generalizedt-Jmodel with dipolar interactions using a system of ultracold fermionic molecules with spin encoded in the two lowest rotational states. We independently tuned the dipolar Ising and spin-exchange couplings and the molecular motion and studied their interplay on coherent spin dynamics. Using Ramsey spectroscopy, we observed and modeled interaction-driven contrast decay that depends strongly both on the strength of the anisotropy between Ising and spin-exchange couplings and on motion. This study paves the way for future exploration of kinetic spin dynamics and quantum magnetism with highly tunable molecular platforms in regimes that are challenging for existing numerical and analytical methods.more » « lessFree, publicly-accessible full text available April 25, 2026
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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.more » « less
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