Understanding Interfacial Nanoparticle Organization through Simulation and Theory: A Review

Abstract

Understanding the behaviors of nanoparticles at interfaces is crucial not only for the design of novel nanostructured materials with superior properties but also for a better understanding of many biological systems where nanoscale objects such as drug molecules, viruses, and proteins can interact with various interfaces. Theoretical studies and tailored computer simulations offer unique approaches to investigating the evolution and formation of structures as well as to determining structure−property relationships regarding the interfacial nanostructures. In this feature article, we summarize our efforts to exploit computational approaches as well as theoretical modeling in understanding the organization of nanoscale objects at the interfaces of various systems. First, we present the latest research advances and state-of-the-art computational techniques for the simulation of nanoparticles at interfaces. Then we introduce the applications of multiscale modeling and simulation methods as well as theoretical analysis to explore the basic science and the fundamental principles in the interfacial nanoparticle organization, covering the interfaces of polymer, nanoscience, biomacromolecules, and biomembranes. Finally, we discuss future directions to signify the framework in tailoring the interfacial organization of nanoparticles based on the computational design. This feature article could promote further efforts toward fundamental research and the wide applications of theoretical approaches in designing interfacial assemblies for new types of functional nanomaterials and beyond.

Seeing the Supracolloidal Assemblies in 3D: Unraveling High-Resolution Structures Using Electron Tomography

“…In this context, computational simulation methods offer valuable information to understand their properties. Various simulation methods, including Monte Carlo, molecular dynamics, mesoscale simulations, self-consistent mean field theory, and ab initio molecular dynamics methods, have been utilized to study the interfacial properties of nanoparticles . The results from computational simulations can be effectively utilized to validate the experimental results using dry-state, liquid-state, and cryo-TEM-tomography-based 3D structures of nanoparticle assemblies.…”

Molecular Dynamics Simulation of the Effects of Complex Surfactants on Oil–Water Interaction and Aggregation Characteristics at the Interface

“…Molecular dynamics (MD) simulation is used to study the arrangement behavior of surfactants, especially the complex system, on the interface and the mechanism of interaction with oil and water at the molecular level, and this process is helpful to effectively understand the oil displacement process and provide theoretical guidance for screening and designing more efficient surfactant. − Zhou found that the sulfuric acid groups of the atomic emission spectroscopy (AES) molecules can attract the DTAC molecules in the mixed surfactants, thereby reducing the repulsion between the molecules. DTAC molecules exhibit excellent molecular interface behavior and can improve the arrangement of AES molecules through the interaction between the headgroups.…”

Janus Ligand-Tethered Nanoparticles at Liquid–Liquid Interfaces

“…Fluid–fluid interfaces involving hairy particles also were extensively investigated. − ,− The surface modification changes the contact angle of particles and their adsorption at the interface. Depending on the nature of attached polymers, the interaction of the particle with a fluid interface can vary from repulsive to attractive.…”

“…Self-assembly of hairy particles at the fluid–fluid interface was also intensively studied. , Numerous experimental works showed that the hairy particles form both disordered monolayers and different 2D structures of a high degree of ordering. − The experimental investigations of the assembly of hairy particles at fluid–fluid interfaces were supported by molecular simulations. − ,, Grest and co-workers carried out atomistic molecular simulations of hairy particles in solutions − and at the liquid–vapor interface. , They observed a spontaneous asymmetry of spherical hairy particles in solutions and at the liquid–vapor interface. They also showed that varying the terminal groups of a nanoparticle canopy strongly alters the coating shape at the water liquid–vapor interface which leads to different assembly morphologies (short linear clusters with a highly aligned structure, dimers, and disordered clumps) .…”