Integration of Periodic External Fields in Dissipative Particle Dynamics Simulation for Designing Stimuli-responsive Triblock Copolymer Materials

Abstract

The development of functionally accurate stimuli-responsive materials based on the principle of dissipative self-assembly (DSA) poses significant challenges within polymer chemistry, a field critical for elucidating the fundamental mechanisms underpinning the specific functions of living organisms. Based on the dissipative particle dynamics simulations, this study proposes a novel approach to driving the DSA process of polymer solutions through the application of periodic external fields, thereby modulating enthalpy changes. We aim to design stimuli-responsive materials capable of dynamically transitioning between non-equilibrium three-dimensional (3D) nanogels and steady-state spherical micelles or layered structures. Our findings indicate that the formation of the dissipative structure of the 3D gel is contingent upon the frequency of the external field exceeding a critical threshold, which instigates high-frequency oscillations of the conformational transitions of the polymer block copolymer. Concurrently, we observe that the power of the external field predominantly influences the formation rate of the dissipative structure; specifically, higher external field power correlates with accelerated formation kinetics. Moreover, the design principle outlined in this research is applicable to polymer concentrations ranging from 20% to 40%, effectively streamlining the experimental procedure by obviating the requirement for precise concentration control. This investigation offers valuable insights into the design of biomimetic stimui-responsive materials and contributes to a deeper understanding of the mechanisms, by which external fields facilitate DSA processes in polymer systems.

Keywords

Block copolymer / Dissipative self-assembly / Dissipative particle dynamics simulation / Stimuli-responsive material

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Jilin University, The Editorial Department of Chemical Research in Chinese Universities and Springer-Verlag GmbH