Quantum state tracking and control of a single molecular ion in a thermal environment

Abstract: Understanding molecular state evolution is central to many disciplines, including molecular dynamics, precision measurement, and molecule-based quantum technology. Details of the evolution are obscured when observing a statistical ensemble of molecules. Here, we reported real-time observations of thermal radiation-driven transitions between individual states ("jumps") of a single molecule. We reversed these "jumps" through microwave-driven transitions, resulting in a twentyfold improvement in the time the molecule dwells in a chosen state. The measured transition rates showed anisotropy in the thermal environment, pointing to the possibility of using single molecules as in-situ probes for the strengths of ambient fields. Our approaches for state detection and manipulation could apply to a wide range of species, facilitating their uses in fields including quantum science, molecular physics, and ion-neutral chemistry.