Interfacial tension and a three-phase generalized self-consistent theory of non-dilute soft composite solids

Abstract: In the dilute limit Eshelby's inclusion theory captures the behavior of a wide range of systems and properties. However, because Eshelby's approach neglects interfacial stress, it breaks down in soft materials as the inclusion size approaches the elastocapillarity length $L$. Here, we use a three-phase generalized self-consistent method to calculate the elastic moduli of composites comprised of an isotropic, linear-elastic compliant solid hosting a spatially random monodisperse distribution of spherical liquid droplets. As opposed to similar approaches, we explicitly capture the liquid-solid interfacial stress when it is treated as an isotropic, strain-independent surface tension. Within this framework, the composite stiffness depends solely on the ratio of the elastocapillarity length $L$ to the inclusion radius $R$. Independent of inclusion volume fraction, we find that the composite is stiffened by the inclusions whenever $R < 3L/2$. Over the same range of parameters, we compare our results with alternative approaches (dilute and Mori-Tanaka theories that include surface tension). Our framework can be easily extended to calculate the composite properties of more general soft materials where surface tension plays a role.