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

Understanding molecular state evolution is central to many disciplines, including molecular dynamics, precision measurement, and molecule-based quantum technology. Details of this evolution are obscured when observing a statistical ensemble of molecules. Here, we report real-time observations of thermal radiation-driven transitions between individual states ("jumps") of a single molecule. We reversed these jumps through microwave-driven transitions, which resulted in a 20-fold 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.