Efficient Cascade Resonance Energy Transfer in Dynamic Nanoassembly for Intensive and Long-Lasting Multicolor Chemiluminescence

Abstract

Light emission induced by chemical reactions, known as chemiluminescence (CL), has been widely used for bioassays, biosensors, imaging, and illumination applications. Most known CL systems exhibit flash-type single-color light emissions, which limit their applications. Long-lasting multicolor CL in aqueous solutions is highly desirable, especially for biological applications, but remains a challenge. Herein, we report a simple strategy of achieving highly efficient cascade Forster resonance energy transfer (FRET) in the dynamic nanoassembly of βcyclodextrin (β-CD), CL reagents, and fluorophores in aqueous solution, which emits intensive multicolor CL with adjustable wavelength within 410−610 nm. β-CD can bind CL reagents and fluorophores to form a dynamic nanoassembly. These nanoassemblies can bring the included luminescent intermediate and fluorophores into close proximity and proper alignment, which should greatly enhance the FRET efficiency between luminescent intermediate and fluorophores. Indeed, the cascade FRET efficiency in this supramolecular nanoassembly reaches up to 92%, which is comparable with the cascade FRET systems based on covalently linked donors and acceptors. By using hydroxypropyl methylcellulose as the thickener to slow the diffusion (to elongate the CL emission), and using Ca(OH) 2 solid (a low solubility strong base) as buffer to maintain the pH in the optimal range for the CL reaction, this nanoassembly system has been further developed to achieve slow-diffusion-controlled catalytic CL reactions, which enables long-lasting multicolor CL in aqueous solution that is visible to naked eyes and lasts for more than 20 h. The multicolor CL systems can be used to prepare transformable two-dimensional multicolor codes for encryption application.

Direct and Indirect Chemiluminescence: Reactions, Mechanisms and Challenges

“…Hydroxypropyl methylcellulose was utilized to slow down the diffusion rate, while the reaction was buffered by addition of solid Ca(OH) 2 . Moreover, it was found that Co 2+ -chitosan increased the CL emission of the system when merged with the β-CD nanoassembly system [126]. Another important study by Lipper et al, described that CL energy transfer from Schaap's dioxetane probe can be efficiently used for ratiometric pH imaging.…”

“…Molecules 2021, 26, 7664 19 of 30 was found that Co 2+ -chitosan increased the CL emission of the system when merged with the β-CD nanoassembly system [126]. Another interesting CL system of cyclic peroxides was catalytically produced by tetrahydrofuran hydrogen peroxide in the presence of BSA-stabilized Gold Nanoclusters (Au@BSA NCs).…”

Quantitative Supramolecular Heterodimerization for Efficient Energy Transfer

“…Energy transfer in a supramolecular system can be readily investigated through steady-state spectroscopic measurements. [61,62] For instance, the complexation of one equivalent of either Np14CMe 2 or Ant910H with two equivalents of CB [7] generates discrete monomers in aqueous solution (Figure 4 a; see Figure S24). [34,36] Their steady-state spectra in Figure 4 c shows that the superposition (the mathematical "mixture") of both monomers spectra (Figure 4 b) resulting in absoroption and emission profiles identical to those recorded for their 50/50 physical mixture.…”

Tuning resonance energy transfer with magneto-optical properties of graphene

“…Different energy transfer mechanisms have been extensively discussed not only in physics, but also in several areas like chemistry, biology and engineering. An efficient energy transfer allows for a variety of applications, such as photovoltaics [6], luminescence [7,8], sensing [9], quantum information [10,11], and many others. Due to these numerous applications and to advances in different areas combined with the great development of new technologies, controlled modification of the RET rate has also become a topic of huge interest.…”

“…Despite its relative simplicity, we could not solve (8) in terms of well known functions. We are, however, particularly interested in the |2iω 0 0 /σ xx | 1/z regime, corresponding to low magnetic fields (away from the abrupt changes at the LL transitions).…”