Omnidispersible Hedgehog Particles with Multilayer Coatings for Multiplexed Biosensing

Hedgehog particles (HPs) replicating the spiky geometry of pollen grains revealed surprisingly high dispersion stability regardless of whether their hydrophobicity/hydrophilicity matches that of the media or not. This property designated as omnidispersibility is attributed to the drastic reduction of van der Waals interactions between particles coated with stiff nanoscale spikes as compared to particles of the same dimensions with smooth surfaces. One may hypothesize but it remains unknown, however, whether HPs modified with polymers or nanoparticles (NPs) would retain this property. Surface modifications of the spikes will expand the functionalities of HPs, making possible their utilization as omnidispersible carriers. Here, we show that HPs carrying dense conformal coatings made by layer-by-layer (LBL/LbL) assembly maintain dispersion stability in environments of extreme polarity and ionic strength. HPs, surface-modified by multilayers of polymers and gold NPs, are capable of surface-enhanced Raman scattering (SERS) and overcome the limited colloidal stability of other SERS probes. The agglomeration resilience of HPs leads to a greater than one order of magnitude increase of SERS intensity as compared to colloids with smooth surfaces and enables simultaneous detection of several targets in complex media with high ionic strength. Omnidispersible optically active colloids open the door for rapid multiplexed SERS analysis in biological fluids and other applications.