Biocompatible Vaterite Carriers Enable Multimodal Quantum Sensing with Nanodiamonds

Abstract

Mobile nanodiamond quantum sensors in liquids are affected by Brownian rotation, variable photon collection, and perturbations from optical trapping. Here we assemble 40-nm nitrogen-vacancy nanodiamonds on porous, birefringent vaterite microspherulites, creating mobile sensors with a polarization-addressable body frame and a chemically active carbonate interface. Under 976-nm trapping, the sensors retain spin resonance and longitudinal relaxation, with less than 7% variation in contrast and an approximately 1-MHz resonance shift at 0.8 W. Zeeman-split resonances resolve magnetic fields from 0 to 0.8 mT, with a response metric of 78--144 $\mu$T Hz${}^{-1/2}$. In cell-culture medium, a 10.7-$\mu$M proton-equivalent dose shortens $T_1$ from $23.4\pm 2.3$ to $9.0\pm 1.2$ $\mu$s, yielding concentration and pH sensitivities of $6.46$ $\mu$M Hz${}^{-1/2}$ and $6.54$ mpH Hz${}^{-1/2}$, respectively. A 500-fold larger proton dose in ethanol produces a weaker response. A grand-canonical charge-regulation model links proton chemical potential to interfacial switching, establishing a route to multimodal quantum sensing in complex liquids.