Mesoscopic structure prediction of nanoparticle assembly and coassembly: Theoretical foundation

Abstract

In this work, we present a theoretical framework that unifies polymer field theory and density functional theory in order to efficiently predict ordered nanostructure formation of systems having considerable complexity in terms of molecular structures and interactions. We validate our approach by comparing its predictions with previous simulation results for model systems. We illustrate the flexibility of our approach by applying it to hybrid systems composed of block copolymers and ligand coated nanoparticles. We expect that our approach will enable the treatment of multi-component self-assembly with a level of molecular complexity that approaches experimental systems.

Linking experiment and theory for three-dimensional networked binary metal nanoparticle–triblock terpolymer superstructures

“…Tick marks in Fig. 1e for this scaling trace show expected peak positions for a G A lattice with I4 1 32 space group, with (q/q 100 ) 2 ¼ 2, 6,8,10,12,14,16,18,20,22,24,26,30,32,34, where the scattering vector q is defined by q ¼ 4 psiny/l, with scattering angle 2y, X-ray wavelength l and reciprocal vector, q 100 , describing the cubic lattice parameter. Expected and observed peak positions match well, suggesting that the SAXS trace of the hybrid is consistent with the G A morphology.…”

“…Here, we demonstrate how the combination of controlled NP synthesis, detailed structural analysis by transmission electron microtomography (TEMT) 15 , energy-dispersive X-ray spectroscopy (EDS) and percolation theory, as well as comparison with a recently developed self-consistent field theory (SCFT) 16,17 enabled highly ordered and porous 3D network formation of single and binary metal NPs from triblock terpolymer self-assembly with particle locations that can be rationalized. Analysis further provided insights into short-and long-range NP-NP correlations, and local and global contributions to structural chirality in an alternating gyroid (G A ) domain.…”

Hairy nanoparticle assemblies as one-component functional polymer nanocomposites: opportunities and challenges

“…Formation of these interconnected networks can be achieved with BCPs, but in the event that one of the functionalities requires an inorganic component, it is necessary to have a library of structures where the nanoparticles are selectively aggregated. BCP-templated nanocomposite structures, in which nanoparticles are forced into specific domains, have been reported both in simulations [44] and experiment, [45][46][47] but they have the same limitations as the conventional nanocomposites mentioned in the introduction (mixing, agglomeration and low inorganic volume fractions). An alternative route is to use HNPs where the hairs are BCPs [48,49] or liquid crystal mesogens [50,51] .…”

Ordering of anisotropic nanoparticles in diblock copolymer lamellae: Simulations with dissipative particle dynamics and a molecular theory

“…38 In the case of polymer nanocomposites the distribution of nanoparticles can be accounted for by combining SCFT with the density functional theory. 39,40 On the other hand, the accuracy of field-based techniques in describing the orientation of the anisotropic particles and, therefore, in predicting the macroscopic anisotropy of the composite is quite limited. As an alternative, hybrid particle-field approaches have been developed [41][42][43] that employ particle-to-field transformation for polymer chains but retain explicit treatment of nanoparticles.…”