Coherent spin-1 dynamics encoded in the rotational states of ultracold molecules

The rotational states of ultracold polar molecules possess long radiative lifetimes, microwave-domain coupling, and tunable dipolar interactions. Coherent dynamics between pairs of rotational states have been used to demonstrate simple models of quantum magnetism and to manipulate quantum information stored as qubits. The availability of numerous rotational states has led to many proposals to implement more complicated models of quantum magnetism, higher-dimensional qudits, and intricate state networks as synthetic dimensions; however, these are yet to be experimentally realised. The primary issue limiting their implementation is the detrimental effect of the optical trapping environment on coherence, which is not easily mitigated for systems beyond two levels. To address this challenge, we investigate the applicability of magic-wavelength optical tweezer traps to facilitate multitransition coherence between rotational states. We demonstrate simultaneous second-scale coherence between three rotational states. Utilising this extended coherence, we perform multiparameter estimation using a generalised Ramsey sequence and demonstrate coherent spin-1 dynamics encoded in the rotational states. Our work paves the way to implementing proposed quantum simulation, computation, and metrology schemes that exploit the rich rotational structure of ultracold polar molecules.