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Principles Of Fluorescence Spectroscopy

There is great need for stand-alone luminescence-based chemosensors that exemplify selectivity, sensitivity, and applicability and that overcome the challenges that arise from complex, real-world media. Discussed herein are recent developments toward these goals in the field of supramolecular luminescent chemosensors, including macrocycles, polymers, and nanomaterials. Specific focus is placed on the development of new macrocycle hosts since 2010, coupled with considerations of the underlying principles of supramolecular chemistry as well as analytes of interest and common luminophores. State-of-the-art developments in the fields of polymer and nanomaterial sensors are also examined, and some remaining unsolved challenges in the area of chemosensors are discussed.

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Supramolecular Luminescent Sensors

Confining molecules can fundamentally change their chemical and physical properties. Confinement effects are considered instrumental at various stages of the origins of life, and life continues to rely on layers of compartmentalization to maintain an out-of-equilibrium state and efficiently synthesize complex biomolecules under mild conditions. As interest in synthetic confined systems grows, we are realizing that the principles governing reactivity under confinement are the same in abiological systems as they are in nature. In this Review, we categorize the ways in which nanoconfinement effects impact chemical reactivity in synthetic systems. Under nanoconfinement, chemical properties can be modulated to increase reaction rates, enhance selectivity and stabilize reactive species. Confinement effects also lead to changes in physical properties. The fluorescence of light emitters, the colours of dyes and electronic communication between electroactive species can all be tuned under confinement. Within each of these categories, we elucidate design principles and strategies that are widely applicable across a range of confined systems, specifically highlighting examples of different nanocompartments that influence reactivity in similar ways.

Chemical reactivity under nanoconfinement

A simple, instrument-free, paper-based analytical device with dual-emission carbon dots (CDs) (blue CDs and red CDs) was developed for the semiquantitative, visual, and sensitive speciation analysis of lead ions in a real sample with a sensitive detection limit of 2.89 nM. When a paper strip was immersed into the sample solution, the blue fluorescence was quenched by Pb2+ in solution, while the red fluorescence served as a background reference without color change, and significant color evolutions from blue to red were observed under the ultraviolet lamp, resulting in a semiquantitative visual detection. Furthermore, a smartphone was used in the visual detection of lead ions by identifying the RGB value of the fluorescent probe solution and corresponding paper strip. The application of smartphones and fluorescent paper strips has greatly shortened the detection time and reduced the cost of detection, providing a new strategy for the on-site and semiquantitative detection of heavy-metal ions in water samples.

Semiquantitative Visual Detection of Lead Ions with a Smartphone via a Colorimetric Paper-Based Analytical Device

A laboratory experiment visually exploring two opposite basic principles of fluorescence of aggregation-caused quenching (ACQ) and aggregation-induced emission (AIE) is demonstrated. The students would prepared two salicylaldehyde-based Schiff bases through a simple one-pot condensation reaction of one equiv of 1,2-diamine with 2 equiv of salicylaldehyde. The resulting fluorescent dyes have similar chemical structures but possess ACQ and AIE properties, respectively. Their ACQ/AIE properties and pH sensing applications would then examined by visually qualitative analysis (UV lamp, light-emitting diode, and naked eye) and quantitative analysis (fluorometer). Finally, in a deeper level, X-ray single crystal structure analysis was utilized to reveal the inherent relationships between molecular structures/molecular arrangements and ACQ/AIE properties. This lesson is suitable for many areas of chemistry, especially for organic and analytical chemistry.

Fluorescence Aggregation-Caused Quenching versus Aggregation-Induced Emission: A Visual Teaching Technology for Undergraduate Chemistry Students

Herein we report a robust and easy method for detecting cesium metal ion (Cs+) in partially aqueous solutions using the fluorescence quenching of 2,4-bis[4-(N,N-dihydroxyethylamino)phenyl]squaraine. This squaraine dye was found to be both highly sensitive (low limits of detection) and selective (limited response to other metals) for cesium ion detection. The detection is likely based on the metal complexing to the dihydroxyethanolamine moieties, which disrupts the donor–acceptor–donor architecture and leads to efficient quenching.

/pdf/sensitive-and-selective-detection-of-cesium-via-fluorescence-32i5p0o3rc.pdf

Sensitive and selective detection of cesium via fluorescence quenching

Reported herein is the immobilization of N-(1-naphthyl)ethylenediamine (NED) on cellulose via an epichlorohydrin (ECH)-based covalent attachment and the implementation of the functionalized cellulo...

https://pubs.acs.org/doi/pdf/10.1021/acssensors.0c01507

Ultrasensitive Detection of Nitrite through Implementation of N-(1-Naphthyl)ethylenediamine-Grafted Cellulose into a Paper-Based Device.

High concentrations of certain nutrients, including phosphate, are known to lead to undesired algal growth and low dissolved oxygen levels, creating deadly conditions for organisms in marine ecosystems. The rapid and robust detection of these nutrients using a colorimetric, paper-based system that can be applied on-site is of high interest to individuals monitoring marine environments and others affected by marine ecosystem health. Several techniques for detecting phosphate have been reported previously, yet these techniques often suffer from high detection limits, reagent instability, and the need of the user to handle toxic reagents. In order to develop improved phosphate detection methods, the commonly used molybdenum blue reagents were incorporated into a paper-based, colorimetric detection system. This system benefited from improved stabilization of the molybdenum blue reagent as well as minimal user contact with toxic reagents. The colorimetric readout from the paper-based devices was analyzed and quantified using RGB analyses (via ImageJ), and resulted in the detection of phosphate at detection limits between 1.3 and 2.8 ppm in various aqueous media, including real seawater.

/pdf/a-paper-based-device-for-ultrasensitive-colorimetric-2p1n2mv6lc.pdf

A Paper-Based Device for Ultrasensitive, Colorimetric Phosphate Detection in Seawater

Reported herein is a new method for the detection of polycyclic aromatic hydrocarbons (PAHs) which relies on energy transfer from the PAH to a near-infrared emitting squaraine fluorophore. This energy transfer occurs inside the γ-cyclodextrin cavity, with up to 35% emission observed from energy transfer compared with exciting the squaraine directly.

Teresa L. Mako

Papers

Supramolecular Luminescent Sensors

Sensitive and selective detection of cesium via fluorescence quenching

Ultrasensitive Detection of Nitrite through Implementation of N-(1-Naphthyl)ethylenediamine-Grafted Cellulose into a Paper-Based Device.

A Paper-Based Device for Ultrasensitive, Colorimetric Phosphate Detection in Seawater

Fluorescent detection of polycyclic aromatic hydrocarbons in ternary cyclodextrin complexes