Direct Nanoparticle Sensing in Liquids with Free-Space Excited Optical Whispering-Gallery-Mode Microresonators

Whispering-gallery-mode (WGM) microresonators are amongst the most promising optical sensors for detecting bio-chemical targets. A number of laser interrogation methods have been proposed and demonstrated over the last decade, based on scattering and absorption losses or resonance splitting and shift, harnessing the high-quality factor and ultra-small volume of WGMs. Actually, regardless of the sensitivity enhancement, their practical sensing operation may be hampered by the complexity of coupling devices as well as the signalprocessing required to extract the WGM response. Here, we use a silica microsphere immersed in an aqueous environment and efficiently excite optical WGMs with a free-space visible laser, thus collecting the relevant information from the transmitted and back-scattered light without any optical coupler, fiber, or waveguide. We show that a 640-nm diode laser, actively frequency-locked on resonance, provides real-time, fast sensing of dielectric nanoparticles approaching the surface with direct analog readout. Thanks to our illumination scheme, the sensor can be kept in water and operate for days without degradation or loss of sensitivity. Diverse noise contributions are carefully considered and quantified in our system, showing a minimum detectable particle size below 1 nm essentially limited by the residual laser microcavity jitter. Further analysis reveals that the inherent laserfrequency instability in the short, -mid-term operation regime sets an ultimate bound of 0.3 nm. Based on this work, we envisage the possibility to extend our method in view of developing new viable approaches for detection of nanoplastics in natural water without resorting to complex chemical laboratory methods.