This critical review introduces a discussion on the influence of preparative procedures (nanofabrication) of nanostructured hybrids and biohybrids, comparing their structural and textural characteristics that determine the properties of the resulting materials. Selected examples of silicate-based hybrids of analogous compositions prepared by both molecular and blocks-assembly bottom–up strategies are discussed to show advantages and inconveniences of each methodology (341 references).

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Hybrid and biohybrid silicate based materials: molecular vs. block-assembling bottom–up processes

The quantitative excited energy transfer reaction between cationic porphyrins on an anionic clay surface was successfully achieved. The efficiency reached up to ca. 100% owing to the “Size-Matching Rule” as described in the text. It was revealed that the important factors for the efficient energy transfer reaction are (i) suppression of the self-quenching between adjacent dyes, and (ii) suppression of the segregated adsorption structure of two kinds of dyes on the clay surface. By examining many different kinds of porphyrins, we found that tetrakis(1-methylpyridinium-3-yl) porphyrin (m-TMPyP) and tetrakis(1-methylpyridinium-4-yl) porphyrin (p-TMPyP) are the suitable porphyrins to accomplish a quantitative energy transfer reaction. These findings indicate that the clay/porphyrin complexes are promising and prospective candidates to be used for construction of an efficient artificial light-harvesting system.

Efficient excited energy transfer reaction in clay/porphyrin complex toward an artificial light-harvesting system.

We have been investigating complexes composed of nanolayered materials with anionic charges such as clay nanosheets and dye molecules such as cationic porphyrins. It was found that the structure of dye assembly on the layered materials can be effectively controlled by the use of electrostatic host–guest interaction. The intermolecular distance, the molecular orientation angle, the segregation/integration behavior, and the immobilization strength of the dyes can be controlled in the clay–dye complexes. The mechanism to control these structural factors has been discussed and was established as a size-matching effect. Unique photochemical reactions such as energy transfer through the use of this methodology have been examined. Almost 100% efficiency of the energy-transfer reaction was achieved in the clay–porphyrin complexes as a typical example for an artificial light-harvesting system. Control of the molecular orientation angle is found to be useful in regulating the energy-transfer efficiency and in prepa...

Size-Matching Effect on Inorganic Nanosheets: Control of Distance, Alignment, and Orientation of Molecular Adsorption as a Bottom-Up Methodology for Nanomaterials

This article provides an insight into state-of-the-art advances in the preparation and functionalization of clay-containing thin films. Layered clay minerals and their synthetic counterparts such as cationic montmorillonite, saponite, laponite and anionic layered double hydroxides are often used as main components or functional fillers in the hybrid films. Strategic assembly of clay minerals or layered double hydroxides with functional molecules has led to a variety of nanostructured clay-containing hybrid films. Frequently used approaches are the solvent casting, the spin-coating, the layer-by-layer (LbL) assembly and the Langmuir–Blodgett (LB) techniques. The type of clay mineral, solvent, pH, organic components and functional molecules generally play a pivotal role in the formation and structure of a desired functional film. Different processes result in differences in the thickness, surface morphology and internal structure in the resultant clay-containing films. Functional polymers, dye molecules, transition metal complexes and protein molecules and even their combination have been exploited to fabricate and functionalize clay-containing films. Many studies have suggested that the functional clay-containing films have potential applications in many areas such as catalysis, modified electrodes and optoelectronic devices, anti-corrosion and packaging materials. Finally, the prospects for the future preparation and applications of clay-containing films are discussed.

Preparation and functionality of clay-containing films

The surface and edge emissions from dye-filled and dye-topped polycarbonate and polymethyl methacrylate luminescent solar concentrators were measured. We demonstrate that about 40-50% of the absorbed light energy (and 50-70% of the photons) is lost through the top and bottom surfaces of the filled waveguide. In most cases the escape cone losses are greater at the top than the bottom surface.

Measured surface loss from luminescent solar concentrator waveguides

In order to elaborate organized two-dimensional arrangements of fluorescent dyes in host solid layered materials, rhodamine 6G (R6G) is encapsulated in supported thin films of laponite (Lap) clay. Clay films are elaborated by the spin-coating technique and their surface morphology is analyzed by scanning electron (SEM) and atomic force (AFM) microscopies. The internal order of the stacked clay layers is checked by X-ray diffraction technique (DRX). The thermostability of R6G in the Lap films is discussed on the basis of several thermogravimetric and calorimetric techniques (TG, DTA and DSC). The R6G adsorbed species in Lap films are characterized by absorption and fluorescence (steady-state and time-resolved) spectroscopies. Monomers, dimers and higher-order aggregates are identified for very low ( 40% of the total cation exchange capacity, CEC, of the clay) dye content, respectively. Both non-fluorescence H-type and fluorescent J-type aggregates of R6G in Lap films are characterized. Absorption and fluorescence techniques with linearly polarized light are applied to evaluate the anisotropic photoresponse of R6G in Lap films, from which the preferential orientation of dye molecules with respect to the clay layers can be evaluated. The validity of the newly established fluorescence polarization is contrasted with the well-established absorption polarization method, and the emission spectroscopy with linearly polarized light can be applied to establish the preferential orientation of fluorophore molecular probes incorporated in any rigid and ordered 2D host materials, including monolayers and biological membranes.

Photoresponse and anisotropy of rhodamine dye intercalated in ordered clay layered films

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Photoresponse and anisotropy of rhodamine dye intercalated in ordered clay layered films