Effect of chain stiffness on the structure of single-chain polymer nanoparticles

被引:19
作者
Moreno, Angel J. [1 ,2 ,3 ]
Bacova, Petra [1 ,2 ,4 ]
Lo Verso, Federica [3 ,5 ]
Arbe, Arantxa [1 ,2 ]
Colmenero, Juan [1 ,2 ,3 ,6 ]
Pomposo, Jose A. [1 ,2 ,6 ,7 ]
机构
[1] Univ Basque Country, CSIC, Paseo Manuel de Lardizabal 5, San Sebastian 20018, Spain
[2] Mat Phys Ctr MPC, Paseo Manuel de Lardizabal 5, San Sebastian 20018, Spain
[3] Donostia Int Phys Ctr, Paseo Manuel de Lardizabal 4, San Sebastian 20018, Spain
[4] Fdn Res & Technol Hellas FORTH, IACM, Iraklion 71110, Greece
[5] Univ Southern Denmark, Dept Phys Chem & Pharm, Campusvej 55, DK-4230 Odense, Denmark
[6] Univ Pais Vasco UPV EHU, Dept Fis Mat, Apartado 1072, E-20800 San Sebastian, Spain
[7] Ikerbasque Basque Fdn Sci, Maria Diaz de Haro 3, Bilbao 48013, Spain
关键词
soft nanoparticles; polymers in solution; computer simulations; INTRINSICALLY DISORDERED PROTEINS; TOPOLOGICAL CONSTRAINTS; CROWDING CONDITIONS; SOFT NANOPARTICLES; WATER; SIMULATIONS; DYNAMICS; DELIVERY; MODEL; MELTS;
D O I
10.1088/1361-648X/aa9f5c
中图分类号
O469 [凝聚态物理学];
学科分类号
070205 ;
摘要
Polymeric single-chain nanoparticles (SCNPs) are soft nano-objects synthesized by purely intramolecular cross-linking of single polymer chains. By means of computer simulations, we investigate the conformational properties of SCNPs as a function of the bending stiffness of their linear polymer precursors. We investigate a broad range of characteristic ratios from the fully flexible case to those typical of bulky synthetic polymers. Increasing stiffness hinders bonding of groups separated by short contour distances and increases looping over longer distances, leading to more compact nanoparticles with a structure of highly interconnected loops. This feature is reflected in a crossover in the scaling behaviour of several structural observables. The scaling exponents change from those characteristic for Gaussian chains or rings in.-solvents in the fully flexible limit, to values resembling fractal or 'crumpled' globular behaviour for very stiff SCNPs. We characterize domains in the SCNPs. These are weakly deformable regions that can be seen as disordered analogues of domains in disordered proteins. Increasing stiffness leads to bigger and less deformable domains. Surprisingly, the scaling behaviour of the domains is in all cases similar to that of Gaussian chains or rings, irrespective of the stiffness and degree of cross-linking. It is the spatial arrangement of the domains which determines the global structure of the SCNP (sparse Gaussian-like object or crumpled globule). Since intramolecular stiffness can be varied through the specific chemistry of the precursor or by introducing bulky side groups in its backbone, our results propose a new strategy to tune the global structure of SCNPs.
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页数:13
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