Contagious Aggregation: Transmittable Protein Aggregation in Cellular Communities Initiated by Synthetic Cells.

Aggregation of amyloidogenic proteins causing neurodegenerative diseases is an uncontrollable and contagious process that is often associated with lipid membranes in a highly complex physiological environment. Although several approaches using natural cells and membrane models have been reported, systematic investigations focusing on the association with the membranes are highly challenging, mostly because of the lack of proper molecular tools. Here, we report a new supramolecular approach using a synthetic cell system capable of controlling the initiation of protein aggregation and mimicking various conditions of lipid membranes, thereby enabling systematic investigations of membrane-dependent effects on protein aggregation by visualization. Extending this strategy through concurrent use of synthetic cells and natural cells, we demonstrate the potential of this approach for systematic and in-depth studies on interrogating inter- and intracellularly transmittable protein aggregation. Thus, this new approach offers opportunities for gaining insights into the pathological implications of contagious protein aggregation associated with membranes for neurotoxicity.

Luminescence Resonance Energy Transfer in a Multiple-Component, Self-Assembled Supramolecular Hydrogel.

Cascade energy transfer from a sensitizer to TbIII then to fluorescent dyes was studied for the first time in a supramolecular hydrogel. Efficient energy transfer from TbIII to the dyes was observed, as established by time-delayed emission and excitation spectral analysis, lifetime data, and microscopic studies.

Ligand Chirality Transfer from Solution State to the Crystalline Self-Assemblies in Circularly Polarized Luminescence (CPL) Active Lanthanide Systems.

The synthesis of a family of chiral and enantiomerically pure pyridyl-diamide (pda) ligands that upon complexation with europium [Eu(CF3SO3)3] result in chiral complexes with metal centered luminescence is reported; the sets of enantiomers giving rise to both circular dichroism (CD) and circularly polarized luminescence (CPL) signatures. The solid-state structures of these chiral metallosupramolecular systems are determined using X-ray diffraction showing that the ligand chirality is transferred from solution to the solid state. This optically favorable helical packing arrangement is confirmed by recording the CPL spectra from the crystalline assembly by using steady state and enantioselective differential chiral contrast (EDCC) CPL Laser Scanning Confocal Microscopy (CPL-LSCM) where the two enantiomers can be clearly distinguished.

Hierarchical supramolecular co-assembly formation employing multi-component light-harvesting charge transfer interactions giving rise to long-wavelength emitting luminescent microspheres.

Charge transfer (CT) interaction induced formation of a hierarchical supramolecular assembly has attracted attention due to its wide diversity of structural and functional characteristics. In the present work, we report the generation of green luminescent microspheres from the charge transfer interaction induced co-assembly of a bis-naphthyl dipicolinic amide (DPA) derivative with tetracyanobenzene (TCNB) for the first time. The properties of these self-assemblies were studied both in solution and the solid-state using spectroscopic and a variety of microscopy techniques. The X-ray crystal structure analysis showed a mixed stack arrangement of DPA and TCNB. The molecular orbital and energy level calculations confirm the charge transfer complex formation between DPA and TCNB. Furthermore, energy transfer was observed from the green luminescent CT complex to a red-emitting dye, pyronin Y, in the microsphere matrix, leading to the formation of a light-harvesting tri-component self-assembly.

Highlights of the development and application of luminescent lanthanide based coordination polymers, MOFs and functional nanomaterials.

The development of lanthanide based coordination polymer and metal-organic framework (CPs and MOFs) nanomaterials as novel functional (e.g. luminescent and magnetic) materials has attracted significant attention in recent times. This is in part due to the wide, but yet unique coordination requirements that the f-metal ions possess, as well as their attractive physical properties, which are often transferred to the bulk material. Hence, there is no surprise, that the design, synthesis and characterisation of lanthanide based CP/MOF materials (featuring either 'pure' lanthanides, or a mixture of both f- and d-metal ions) for applications in gas and small molecule absorption, storage, conversion/catalysis, chemical sensing, bio-imaging, drug delivery, etc. has been a prominent feature in the scientific literature. In this review, we give a selected overview of some of the recent developments in the area of Ln CP/MOF based nanomaterials for sensing, optical materials and bio-medicine research, as well as making reference to some more established examples, with the view of introducing, particularly to new researchers to the field, the powerful and attractive features of lanthanide based materials.

An Inexpensive Paper-Based Photoluminescent Sensor for Gallate Derived Green Tea Polyphenols.

This work describes a terbium luminescence-based protocol to selectively detect gallate-derived green tea polyphenols on a supramolecular gel immobilised paper platform for the first time. This user-friendly, inexpensive (€â€…0.0015) approach requires very low sample volumes for the analysis. The developed strategy enables simultaneous detection of gallate polyphenols in multiple tea samples with the potential for practical applications.

Eu/Tb luminescence for alkaline phosphatase and ß-galactosidase assay in hydrogels and on paper devices.

Simple technologies for efficient detection of important (bio)molecules are always in great demand. We now report the detection and assay of two biologically important enzymes, alkaline phosphatase and ß-galactosidase, in Eu- or Tb-based cholate hydrogels, respectively, and on filter paper discs coated with such hydrogels. Pro-sensitizers derived from 1-hydroxypyrene and 2,3-dihydroxynaphthalene were incorporated into Eu or Tb cholate hydrogels, respectively. Upon enzyme action, these artificial substrates liberate free sensitizers both in the gel and on gel-coated discs, resulting in turn-on luminescence, red/magenta for Eu, and green for Tb. The detection of enzymes was also demonstrated in natural/biological samples using low-cost systems.