Structure and dynamics of single-chain nano-particles in solution

被引：45

作者：

Arbe, A. ^{[1
]}

Pomposo, J. A. ^{[1
,2
,3
]}

Moreno, A. J. ^{[1
]}

LoVerso, F. ^{[1
]}

Gonzalez-Burgos, M. ^{[1
]}

Asenjo-Sanz, I. ^{[1
]}

Iturrospe, A. ^{[1
]}

Radulescu, A. ^{[4
]}

Ivanova, O. ^{[4
]}

Colmenero, J. ^{[1
,2
,5
]}

机构：

[1] CFM CSIC UPV EHU, MPC, Paseo Manuel de Lardizabal 5, San Sebastian 20018, Spain

[2] Dept Fis Mat UPV EHU, Apartado 1072, San Sebastian 20080, Spain

[3] Basque Fdn Sci, Ikerbasque, Maria Diaz de Haro 3, Bilbao 48013, Spain

[4] Forschungszentrum Julich, JCNS, Heinz Maier Leibnitz Zentrum MLZ, Lichtenbergstr 1, D-85748 Garching, Germany

[5] Donostia Int Phys Ctr, Paseo Manuel de Lardizabal 4, San Sebastian 20018, Spain

来源：

POLYMER | 2016年 / 105卷

基金：

欧盟第七框架计划;

关键词：

Single-chain nano-particles; Small angle scattering; Quasielastic neutron scattering; Molecular dynamics simulations; NEUTRON SPIN-ECHO; INTRINSICALLY DISORDERED PROTEINS; POLYMER NANOPARTICLES; SCATTERING; COVALENT; NONCOVALENT; MODEL;

D O I：

10.1016/j.polymer.2016.07.059

中图分类号：

O63 [高分子化学（高聚物）];

学科分类号：

070305 ; 080501 ; 081704 ;

摘要：

By means of intramolecular folding/collapse of individual polymer chains (precursors), ultra-small soft nano-objects called single-chain nano-particles (SCNPs) can be synthesized. Here we present a combination of scattering techniques [small angle X-Ray and neutron scattering (SAXS and SANS), neutron spin echo (NSE) and dynamic light scattering (DLS)] to investigate the structure and dynamics of SCNPs in solution and their linear precursors as reference. Coarse-grained molecular dynamics (MD) simulations have also been carried out to complement this study. The application of SANS and SAXS has proved the compaction of the macromolecules upon creation of internal cross-links. However, the SCNPs obtained by different routes exhibit a far from globular topology in good solvent. Regarding the dynamics, we report on the first experimental investigation of the dynamic structure factor of SCNPs in solution. It reveals a clear impact of internal cross-links through (i) a reduction of the translational diffusion coefficient and (ii) an important slowing down of the internal modes. The data have been analyzed in terms of theoretical approximations based on the Zimm model. Both, structurally and dynamically, SCNPs show striking resemblances with intrinsically disordered proteins: similar scaling properties reflecting sparse morphologies and an extremely high internal friction. (C) 2016 Elsevier Ltd. All rights reserved.

引用

页码：532 / 544

页数：13

共 50 条

[1]

ALLEGRA G, 1989, ADV CHEM PHYS, V75, P265

[2] Single-Chain Folding of Synthetic Polymers: A Critical Update [J].

Altintas, Ozcan ;

Barner-Kowollik, Christopher .

MACROMOLECULAR RAPID COMMUNICATIONS, 2016, 37 (01) :29-46

[3] Single Chain Folding of Synthetic Polymers by Covalent and Non-Covalent Interactions: Current Status and Future Perspectives [J].

Altintas, Ozcan ;

Barner-Kowollik, Christopher .

MACROMOLECULAR RAPID COMMUNICATIONS, 2012, 33 (11) :958-971

[4] Origin of internal viscosity effects in flexible polymers: A comparative neutron spin-echo and light scattering study on poly(dimethylsiloxane) and polyisobutylene [J].

Arbe, A ;

Monkenbusch, M ;

Stellbrink, J ;

Richter, D ;

Farago, B ;

Almdal, K ;

Faust, R .

MACROMOLECULES, 2001, 34 (05) :1281-1290

[5] Neutron scattering and molecular dynamics simulations: synergetic tools to unravel structure and dynamics in polymers [J].

Arbe, Arantxa ;

Alvarez, Fernando ;

Colmenero, Juan .

SOFT MATTER, 2012, 8 (32) :8257-8270

[6]

Artar M., 2014, ACS S SERIES

[7]

Bernado A P, 2012, ROYAL SOC CHEM, V8, P151, DOI [10.1039/c1mb05275f, DOI 10.1039/C1MB05275F]

[8] Direct observation of correlated interdomain motion in alcohol dehydrogenase [J].

Biehl, Ralf ;

Hoffmann, Bernd ;

Monkenbusch, Michael ;

Falus, Peter ;

Preost, Sylvain ;

Merkel, Rudolf ;

Richter, Dieter .

PHYSICAL REVIEW LETTERS, 2008, 101 (13)

[9]

Doi M., 1988, The Theory of Polymer Dynamics

[10]

Ewen B, 1997, ADV POLYM SCI, V134, P1

← 1 2 3 4 5 →