Title: Correlating microscopic viscoelasticity and structure of an aging colloidal gel using active microrheology and cryogenic scanning electron microscopy

Abstract: Optical tweezers (OTs) can detect pico-Newton range forces operating on a colloidal particle trapped in a medium and have been successfully utilized to investigate complex systems with internal structures. Laponite clay particles in an aqueous medium self-assemble to form microscopic networks over time as electrostatic interactions between the particles gradually evolve in a physical aging process. We investigate the forced movements of an optically trapped micron-sized colloidal probe particle, suspended in an aging Laponite suspension, as the underlying Laponite microstructures gradually develop. Our OT-based oscillatory active microrheology experiments allow us to investigate the mechanical responses of the evolving microstructures in aging aqueous clay suspensions of concentrations ranging from 2.5% w/v to 3.0% w/v and at several aging times between 90 and 150 minutes. We repeat such oscillatory measurements for a range of colloidal probe particle diameters and investigate the effect of probe size on the microrheology of the aging suspensions. Using cryogenic field emission scanning electron microscopy (cryo-FESEM), we examine the average pore areas of the Laponite suspension microstructures for various sample concentrations and aging times. By combining our OT and cryo-FESEM data, we report here for the first time to the best of our knowledge, an inverse correlation between the crossover modulus and the average pore diameter of the aging suspension microstructures for the different suspension concentrations and probe particle sizes studied here.