Molecular self-assembly is the spontaneous association of molecules under equilibrium conditions into stable, structurally well-defined aggregates joined by noncovalent bonds. Molecular self-assembly is ubiquitous in biological systems and underlies the formation of a wide variety of complex biological structures. Understanding self-assembly and the associated noncovalent interactions that connect complementary interacting molecular surfaces in biological aggregates is a central concern in structural biochemistry. Self-assembly is also emerging as a new strategy in chemical synthesis, with the potential of generating nonbiological structures with dimensions of 1 to 10(2) nanometers (with molecular weights of 10(4) to 10(10) daltons). Structures in the upper part of this range of sizes are presently inaccessible through chemical synthesis, and the ability to prepare them would open a route to structures comparable in size (and perhaps complementary in function) to those that can be prepared by microlithography and other techniques of microfabrication.

Molecular self-assembly and nanochemistry: A chemical strategy for the synthesis of nanostructures

Magnetocaloric effect: From materials research to refrigeration devices

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Theory Of Simple Liquids

Colloidal nanocrystals are nanometer-sized, solution-grown inorganic particles stabilized by a layer of surfactants attached to their surface. The inorganic cores exhibit useful properties controlled by composition as well as size and shape, while the surfactant coating ensures that these structures are easy to fabricate and process. It is this combination of features that makes colloidal nanocrystals attractive and promising building blocks for advanced materials and devices. But their full potential can only be exploited if we achieve exquisite control over their composition, size, shape, crystal structure and surface properties. Here we review what is known about nanocrystal growth and outline strategies for controlling it.

Colloidal nanocrystal synthesis and the organic-inorganic interface

The self-assembly of inorganic nanoparticles is of great importance in realizing their enormous potentials for broad applications due to the advanced collective properties of nanoparticle ensembles. Various molecular ligands (e.g., small molecules, DNAs, proteins, and polymers) have been used to assist the organization of inorganic nanoparticles into functional structures at different hierarchical levels. Among others, polymers are particularly attractive for use in nanoparticle assembly, because of the complex architectures and rich functionalities of assembled structures enabled by polymers. Polymer-guided assembly of nanoparticles has emerged as a powerful route to fabricate functional materials with desired mechanical, optical, electronic or magnetic properties for a broad range of applications such as sensing, nanomedicine, catalysis, energy storage/conversion, data storage, electronics and photonics. In this review article, we summarize recent advances in the polymer-guided self-assembly of inorganic nanoparticles in both bulk thin films and solution, with an emphasis on the role of polymers in the assembly process and functions of resulting nanostructures. Precise control over the location/arrangement, interparticle interaction, and packing of inorganic nanoparticles at various scales are highlighted.

Polymer-guided assembly of inorganic nanoparticles.

We describe a robust method to assemble nanoparticles into highly ordered superlattices by inducing aqueous phase separation of neutral capping polymers. Here we demonstrate the approach with thiolated polyethylene-glycol-functionalized gold nanoparticles (PEG-AuNPs) in the presence of salts (for example, K2CO3) in solutions that spontaneously migrate to the liquid–vapor interface to form a Gibbs monolayer. We show that by increasing salt concentration, PEG-AuNP monolayers transform from two-dimensional (2D) gas-like to liquid-like phase and eventually, beyond a threshold concentration, to a highly ordered hexagonal structure, as characterized by surface sensitive synchrotron X-ray reflectivity and grazing incidence X-ray diffraction. Furthermore, the method allows control of the inplane packing in the crystalline phase by varying the K2CO3 and PEG-AuNPs concentrations and the length of PEG. Using polymer-brush theory, we argue that the assembly and crystallization is driven by the need to reduce surface tension between PEG and the salt solution. Our approach of taking advantage of the phase separation of PEG in salt solutions is general (i.e., can be used with any nanoparticles) leads to high-quality macroscopic and tunable crystals. Finally, we discuss how the method can also be applied to the design of orderly 3D structures.

https://lib.dr.iastate.edu/cgi/viewcontent.cgi?article=1001&context=ameslab_manuscripts

Macroscopic and tunable nanoparticle superlattices

Taking advantage of the aqueous biphasic behavior of polyethylene glycol (PEG)/salts, recent experiments have demonstrated self-assembly and crystallization of PEG-grafted gold nanoparticles (PEG-AuNPs) into tunable two-dimensional (2D) supercrystals by adjusting salt concentration (for instance, K2CO3). In those studies, combined experimental evidence and theoretical analysis have pointed out the possibility that similar strategies can lead to three-dimensional (3D) formation of ordered nanoparticle precipitates. Indeed, a detailed small-angle X-ray scattering (SAXS) study reported herein reveals the spontaneous formation of PEG-AuNPs assemblies in high-concentration salt solutions that exhibit short-range 3D order compatible with fcc symmetry. We argue that the assembly into fcc crystals is driven by partnering nearest-neighbors to minimize an effective surface-tension gradient at the boundary between the polymer shell and the high-salt media. We report SAXS and other results on PEG-AuNPs of various Au core diameters in the range of 10 to 50 nm and analyze them in the framework of brush-polymer theory revealing a systematic prediction of the nearest-neighbor distance in the 3D assemblies.

Assembling and ordering polymer-grafted nanoparticles in three dimensions.

https://lib.dr.iastate.edu/cgi/viewcontent.cgi?article=1314&context=cbe_pubs

Synthesis and characterization of Gd-doped magnetite nanoparticles

Nanoparticle-based clusters permit the harvesting of collective and emergent properties, with applications ranging from optics and sensing to information processing and catalysis. However, existing approaches to create such architectures are typically system-specific, which limits designability and fabrication. Our work addresses this challenge by demonstrating that cluster architectures can be rationally formed using components with programmable valence. We realize cluster assemblies by employing a three-dimensional (3D) DNA meshframe with high spatial symmetry as a site-programmable scaffold, which can be prescribed with desired valence modes and affinity types. Thus, this meshframe serves as a versatile platform for coordination of nanoparticles into desired cluster architectures. Using the same underlying frame, we show the realization of a variety of preprogrammed designed valence modes, which allows for assembling 3D clusters with complex architectures. The structures of assembled 3D clusters are verified by electron microcopy imaging, cryo-EM tomography and in-situ X-ray scattering methods. We also find a close agreement between structural and optical properties of designed chiral architectures.

/pdf/valence-programmable-nanoparticle-architectures-24um0ez3h3.pdf

Valence-programmable nanoparticle architectures.

Ion-specific effects on the assembly and crystallization of polyethylene-glycol-grafted Au nanoparticles (PEG-AuNPs) at the vapor–liquid interface are examined by surface sensitive synchrotron X-ray scattering methods. We show that monovalent salts, such as KCl and NaCl, that do not advance phase separation of pure PEG at room temperature induce two-dimensional (2D) self-assembly and crystallization of PEG-AuNPs with some distinctions. Whereas for KCl the 2D hexagonal coherence length of the PEG-AuNP superlattices is remarkably large compared to other salts (over micron-sized crystalline grains), NaCl induces coexistence of two hexagonal structures. Using various salts, we find that the value of the lattice constant is correlated to the ionic hydration entropy consistent with the Hofmeister series.

Honghu Zhang

Papers

Macroscopic and tunable nanoparticle superlattices

Assembling and ordering polymer-grafted nanoparticles in three dimensions.

Synthesis and characterization of Gd-doped magnetite nanoparticles

Valence-programmable nanoparticle architectures.

Ion-Specific Interfacial Crystallization of Polymer-Grafted Nanoparticles