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Polymeric single-chain nanoparticles (SCNPs) are soft nano-objectssynthesized by purely intramolecular cross-linking of single polymer chains. Bymeans of computer simulations, we investigate the conformational properties ofSCNPs as a function of the bending stiffness of their linear polymerprecursors. We investigate a broad range of characteristic ratios from thefully flexible case to those typical of bulky synthetic polymers. Increasingstiffness hinders bonding of groups separated by short contour distances andincreases looping over longer distances, leading to more compact nanoparticleswith a structure of highly interconnected loops. This feature is reflected in acrossover in the scaling behaviour of several structural observables. Thescaling exponents change from those characteristic for Gaussian chains or ringsin $\theta$-solvents in the fully flexible limit, to values resembling fractalor `crumpled' globular behaviour for very stiff SCNPs. We characterize domainsin the SCNPs. These are weakly deformable regions that can be seen asdisordered analogues of domains in disordered proteins. Increasing stiffnessleads to bigger and less deformable domains. Surprisingly, the scalingbehaviour of the domains is in all cases similar to that of Gaussian chains orrings, irrespective of the stiffness and degree of cross-linking. It is thespatial arrangement of the domains which determines the global structure of theSCNP (sparse Gaussian-like object or crumpled globule). Since intramolecularstiffness can be varied through the specific chemistry of the precursor or byintroducing bulky side groups in its backbone, our results propose a newstrategy to tune the global structure of SCNPs.

Effect of Chain Stiffness on the Structure of Single-Chain Polymer Nanoparticles