“…The influence of particle morphology on adhesive performance has already been studied by Aymonier et al20–22 However, no special effort to control molecular weight and gel fraction of both phases was made, and in that case not much improvement was obtained using a heterogeneous morphology or a gradient composition compared to a homogeneous one. The heterogeneous structure of Aymonier et al21 shows e.g., a lack of adhesion and cohesion probably because the composition of each phase, outer and within the particle, is not optimized for this type of structure. More recently Deplace, Foster and coworkers have explored this concept of heterogeneous particle in more detail and in addition to the structure of the particle itself,19, 23–25 have focused also on the synergy between particle structure and polymer architecture and saw a clear improvement in macroscopic adhesive properties.…”