Non-equilibrium self-assembly processes: thermodynamics of structures formation out of equilibrium

In nature, we can find self-organized systems from the size of a few atoms to the cosmologic scale. The structures found in self-organized systems are formed by non-equilibrium processes, in which matter and energy are dissipated. On the other hand, the simplest self-organized systems are those without feedback loops, in which self-assembled structures are formed. In the present work, a general mechanism non-equilibrium self-assembled structures with defined architecture is formulated with the purpose to describe thermodynamically the self-assembly process out of equilibrium in the mesoscale and to evaluate the thermodynamic viability of the structures. Therefore, we define the fundamental building block, the order of the structures and the fundamental sub-processes that compose the non-equilibrium self-assembly process. Once this is defined, a mathematical model is developed, obtaining a system of Fokker-Planck equations which describe the intermediate structures in the self-assembly process. The model is validated from experimental data found in the literature. The gelation process and the Liesegang-type pattern formation process are taken as case studies for the model validation. Also, the conjecture of the minimum change in the total entropy generated is formulated, which allows us to relate the thermodynamic viability of the possible self-assembled structures with the total entropy produced for their formation. Here the conjecture is confirmed for the case studies mentioned above, gelation and Liesegang type patterns. From the mechanism, the model and the proposed conjecture, several self-assembled and even self-organized systems could be studied. In addition, the present work opens a new window for the analysis, control, and optimization of self-assembled structures in the fields of materials science, nano-technology and biophysics. Finally, from the proposed conjecture, we obtain an alternative approach for the evolution in self-organized systems, since this non-Darwinian model describes the evolution driven by dissipative forces.

• Autores: Arango-Restrepo, Andrés
• Fecha de publicación: 2017
• Institución: Universidad Nacional de Colombia
• Repositorio: Universidad Nacional de Colombia
• Idioma: spa
• OAI Identifier: oai:repositorio.unal.edu.co:unal/69034
• Acceso en línea: https://repositorio.unal.edu.co/handle/unal/69034; http://bdigital.unal.edu.co/70444/
• Palabra clave: 54 Química y ciencias afines / Chemistry; out-of-equilibrium; kinetics; self-assembly; entropy production; dissipation; processes; Procesos de no-equilibrio; Termodinámica; Meso-estructuras; Evolución molecular; Química Química supramolecular
• Rights: openAccess
• License: Atribución-NoComercial 4.0 Internacional