Cascade Förster resonance energy transfer between layered silicate edge-linked chromophores

Förster resonance energy transfer (FRET) serves as a critical mechanism to study intermolecular interactions and the formation of macromolecular assemblies. Cascade FRET is a multi-step FRET process which can overcome limitations associated with traditional single-step FRET. Herein, a novel organic-inorganic hybrid composed of a nile red derivative attached to the edge of the layered silicate clay Laponite (Lap-NR) was used to facilitate cascade FRET between Laponite sheets. Utilizing naphthalene-diimide edge-modified Laponite (Lap-NDI) as the initial donor, Rhodamine 6G on the basal surface of Laponite as the first acceptor, and Lap-NR as the second acceptor, cascade FRET was achieved. The influence of solvent composition in a DMF/water mixture on cascade FRET was investigated, revealing that a higher water content led to an enhancement of the cascade FRET process, which is attributed to increased aggregation-induced emission of Lap-NDI and the enhanced quantum yield of R6G in water. This study provides a unique approach to achieve cascade FRET by taking advantage of the anisotropic surface chemistry of a two-dimensional nanomaterial, providing a colloidally-driven alternative with improved tunability compared to macromolecular routes. The flexibility and simplicity of this approach will advance the state of the art of organic-inorganic hybrids for applications in optoelectronics, sensors, and hybrid photovoltaics.