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Hollow microgels, consisting of a pNIPAM polymer network with a centralcavity, have significant potential due to their tunable softness andencapsulation capabilities. Using molecular dynamics simulations, we thoroughlycharacterise the swelling behaviour of neutral hollow microgels across theVolume Phase Transition (VPT) upon varying crosslinker concentration, shellthickness, and size. In particular, we examine in detail the onset of cavityfilling and its relation to the VPT, detecting the presence of a discontinuityin the radius of gyration of the microgels, if an appropriate balance betweenshell stiffness and thermoresposiveness is reached. The discontinuity is,however, absent in the behaviour of the hydrodynamic radius, in agreement withexperimental observations. We then test our numerical model by directcomparison of form factors with available measurements in the literature andalso establish a minimal-size, stable hollow microgel for futurecomputationally feasible bulk investigations. Overall, our findings providevaluable insights into the fundamental swelling properties of hollow microgelsthat can be useful to control the opening and closing of the cavity forapplication purposes.

Numerical insights on the volume phase transition of thermoresponsive hollow microgels