Ultrafast, all-optical coherence of molecular electron spins in room-temperature, aqueous solution

The tunability and spatial precision of paramagnetic molecules makes them attractive for quantum sensing. However, usual microwave-based detection methods have poor temporal and spatial resolution, and optical methods compatible with room-temperature solutions have remained elusive. Here, we utilize pump-probe polarization spectroscopy to initialize and track electron spin coherence in a molecule. Designed to efficiently couple spins to light, aqueous K₂IrCl₆ enables detection of few-picosecond free induction decay at room temperature and micromolar concentrations. Viscosity is found to strongly vary decoherence lifetimes. This work redefines the meaning of room-temperature coherence by improving experimental time resolution by up to five orders of magnitude. Doing so unveils a new regime of electron spin coherence, opening the door to new synthetic design and applications of molecular quantum bits.