Liquid photonic-molecule microlasers for ultrasensitive biosensing

Droplet microlasers, as promising tools for biophotonics and biomedical sciences, have witnessed rapid advances due to their flexible reconfigurability, high sensitivity to stimuli, and label-free biosensing ability. However, designing these biosensors with simultaneously critical properties of low lasing threshold, high spectral purity, and ultimate sensitivity remains challenging. Here, we propose a versatile strategy to build liquid photonic molecules (LPMs) that combine all these features in a single device. We find that through tailoring the spectral Vernier overlap in size-mismatched droplets, this device enables single-mode lasing with a low threshold of ~610 nJ mm-2. The LPM lasers are engineered for dynamic tunability using a molecular isomerization strategy, which induces spectral mode hopping and thus yields a nearly ten-fold enhancement in spectral sensitivity over single droplets. Moreover, by leveraging the self-referenced intensity response of the LPM lasing modes, we demonstrate a three-orders-of-magnitude enhancement in biomolecular sensing, with a detection limit of 30 aM and a dynamic range spanning nine orders of magnitude. Our work offers exciting prospects for bio-integrated liquid sensors in diverse applications.