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Polymers
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Current Directions and Innovations in Fluorescence Techniques for Characterization of...
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Current Directions and Innovations in Fluorescence Techniques for Characterization of Polymers and Polymeric Materials

A special issue of Polymers (ISSN 2073-4360). This special issue belongs to the section "Polymer Analysis and Characterization".

Deadline for manuscript submissions: closed (30 August 2023) | Viewed by 6928

Special Issue Editor

Prof. Dr. Jean Duhamel

E-Mail Website
Guest Editor
Institute for Polymer Research, Waterloo Institute of Nanotechnology, Department of Chemistry, University of Waterloo, Waterloo, ON N2L 3G1, Canada
Interests: fluorescence; polymer science; polypeptides; polysaccharides; polymeric bottle brushes
Special Issues, Collections and Topics in MDPI journals

Special Issue Information

Dear Colleagues,

The ability of fluorescent dyes to sense their surroundings over a few nanometers enables fluorescence experiments to probe soft matter at the molecular level. This feature makes fluorescence a well-suited technique to characterize the structure and dynamics of macromolecules. Such studies are facilitated by its outstanding sensitivity, enabling the fluorescently labeled macromolecule to be investigated with a minimal number of probes, thus ensuring that its properties are minimally affected by the presence of dye(s), and at infinitely low concentrations of a few mg/L, enabling the study of individual macromolecules. While most fluorescence experiments revolve around fluorescence quenching, fluorescence resonance energy transfer (FRET), or fluorescence anisotropy, new fluorescence-based methodologies are constantly being introduced to expand the type of information describing the properties of polymeric materials. This Special Issue aims to introduce current directions and innovations for the application of fluorescence techniques to the study of polymeric materials.

Prof. Dr. Jean Duhamel
Guest Editor

Manuscript Submission Information

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Submitted manuscripts should not have been published previously, nor be under consideration for publication elsewhere (except conference proceedings papers). All manuscripts are thoroughly refereed through a single-blind peer-review process. A guide for authors and other relevant information for submission of manuscripts is available on the Instructions for Authors page. Polymers is an international peer-reviewed open access semimonthly journal published by MDPI.

Please visit the Instructions for Authors page before submitting a manuscript. The Article Processing Charge (APC) for publication in this open access journal is 2700 CHF (Swiss Francs). Submitted papers should be well formatted and use good English. Authors may use MDPI's English editing service prior to publication or during author revisions.

Keywords

  • fluorescence
  • polymers
  • length scales
  • dynamics
  • structure
  • imaging

Published Papers (5 papers)

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Research

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16 pages, 2031 KiB  
Article
Multifunctional Nanoparticles with Superparamagnetic Mn(II) Ferrite and Luminescent Gold Nanoclusters for Multimodal Imaging
by Bárbara Casteleiro, Mariana Rocha, Ana R. Sousa, André M. Pereira, José M. G. Martinho, Clara Pereira and José P. S. Farinha
Polymers 2023, 15(22), 4392; https://doi.org/10.3390/polym15224392 - 13 Nov 2023
Viewed by 780
Abstract
Gold nanoclusters (AuNCs) with fluorescence in the Near Infrared (NIR) by both one- and two-photon electronic excitation were incorporated in mesoporous silica nanoparticles (MSNs) using a novel one-pot synthesis procedure where the condensation polymerization of alkoxysilane monomers in the presence of the AuNCs [...] Read more.
Gold nanoclusters (AuNCs) with fluorescence in the Near Infrared (NIR) by both one- and two-photon electronic excitation were incorporated in mesoporous silica nanoparticles (MSNs) using a novel one-pot synthesis procedure where the condensation polymerization of alkoxysilane monomers in the presence of the AuNCs and a surfactant produced hybrid MSNs of 49 nm diameter. This method was further developed to prepare 30 nm diameter nanocomposite particles with simultaneous NIR fluorescence and superparamagnetic properties, with a core composed of superparamagnetic manganese (II) ferrite nanoparticles (MnFe2O4) coated with a thin silica layer, and a shell of mesoporous silica decorated with AuNCs. The nanocomposite particles feature NIR-photoluminescence with 0.6% quantum yield and large Stokes shift (290 nm), and superparamagnetic response at 300 K, with a saturation magnetization of 13.4 emu g−1. The conjugation of NIR photoluminescence and superparamagnetic properties in the biocompatible nanocomposite has high potential for application in multimodal bioimaging. Full article
(This article belongs to the Special Issue Current Directions and Innovations in Fluorescence Techniques for Characterization of Polymers and Polymeric Materials)
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20 pages, 8737 KiB  
Article
Persistence Length of PEGMA Bottle Brushes Determined by Pyrene Excimer Fluorescence
by Janine L. Thoma, Hunter Little, Jean Duhamel, Lei Zhang and Kam Tong Leung
Polymers 2023, 15(19), 3958; https://doi.org/10.3390/polym15193958 - 30 Sep 2023
Cited by 2 | Viewed by 695
Abstract
Seven pyrene-labeled poly(oligo(ethylene glycol) methyl ether methacrylate)s (PyEG5-PEGnMAs) were prepared with n = 0, 3, 4, 5, 7, 9, and 19 ethylene glycol units by copolymerizing a small amount of penta(ethylene glycol) 1-pyrenemethyl ether methacrylate with an EGn [...] Read more.
Seven pyrene-labeled poly(oligo(ethylene glycol) methyl ether methacrylate)s (PyEG5-PEGnMAs) were prepared with n = 0, 3, 4, 5, 7, 9, and 19 ethylene glycol units by copolymerizing a small amount of penta(ethylene glycol) 1-pyrenemethyl ether methacrylate with an EGnMA monomer. The conformation of the PyEG5-PEGnMA polymers evolved from a random coil for PyEG5-PEG0MA or poly(methyl methacrylate) to a polymeric bottle brush (PBB) architecture with increasing side chain length. The fluorescence decays of the PyEG5-PEGnMA samples were fitted according to the fluorescence blob model (FBM) whose parameters were used, in combination with the Kratky–Porod equation, to calculate the persistence length of these polymers. The persistence lengths obtained from the PEF experiments were found to increase with the square of the number (NS) of non-hydrogen atoms in the side chain as expected theoretically. The persistence lengths found with the PyEG5-PEGnMA samples in DMF also matched those found earlier for another series of PEGnMA samples labeled with 1-pyrenebutanol. The good agreement found between the persistence lengths obtained with the PEGnMA samples labeled with two different pyrene derivatives illustrates the robustness of the method and its applicability for measuring the unknown persistence length of polydisperse polymer samples. Full article
(This article belongs to the Special Issue Current Directions and Innovations in Fluorescence Techniques for Characterization of Polymers and Polymeric Materials)
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13 pages, 2316 KiB  
Article
Facile Obtainment of Fluorescent PEG Hydrogels Bearing Pyrene Groups by Frontal Polymerization
by Ricardo D. Martínez-Serrano, Fabián Cuétara-Guadarrama, Mireille Vonlanthen, Javier Illescas, Xiao-Xia Zhu and Ernesto Rivera
Polymers 2023, 15(7), 1687; https://doi.org/10.3390/polym15071687 - 28 Mar 2023
Cited by 1 | Viewed by 1432
Abstract
Frontal polymerization (FP) was used to prepare poly(ethylene glycol) methyl ether acrylate (PEGMA) fluorescent polymer hydrogels containing pyrenebutyl pendant groups as fluorescent probes. The polymerization procedure was carried out under solvent-free conditions, with different molar quantities of pyrenebutyl methyl ether methacrylate (PybuMA) and [...] Read more.
Frontal polymerization (FP) was used to prepare poly(ethylene glycol) methyl ether acrylate (PEGMA) fluorescent polymer hydrogels containing pyrenebutyl pendant groups as fluorescent probes. The polymerization procedure was carried out under solvent-free conditions, with different molar quantities of pyrenebutyl methyl ether methacrylate (PybuMA) and PEGMA, in the presence of tricaprylmethylammonium (Aliquat 336®) persulfate as a radical initiator. The obtained PEGPy hydrogels were characterized by FT-IR spectroscopy, confirming the effective incorporation of the PybuMA monomer into the polymer backbone. The thermal properties of the hydrogels were determined using thermogravimetric analysis (TGA) and differential scanning calorimetry (DSC). After immersing the hydrogels in deionized water at 25 °C and pH = 7, their swelling behavior was investigated by mass gain at different pH and temperature values. The introduction of PybuMA comonomer into the hydrogel resulted in a decreased swelling ability due to the hydrophobicity of PybuMA. The optical properties of PEGPy were determined by UV-visible absorption and fluorescence spectroscopies. Both monomer and excimer emission bands were observed at 379–397 and 486 nm, respectively, and the fluorescence spectra of the PEGPy hydrogel series were recorded in different solvents to explore the coexistence of monomer and excimer emissions. Full article
(This article belongs to the Special Issue Current Directions and Innovations in Fluorescence Techniques for Characterization of Polymers and Polymeric Materials)
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19 pages, 2804 KiB  
Article
Diffusion-Enhanced Förster Resonance Energy Transfer in Flexible Peptides: From the Haas-Steinberg Partial Differential Equation to a Closed Analytical Expression
by Maik H. Jacob, Roy N. D’Souza, Alexandra I. Lazar and Werner M. Nau
Polymers 2023, 15(3), 705; https://doi.org/10.3390/polym15030705 - 30 Jan 2023
Cited by 3 | Viewed by 2677
Abstract
In the huge field of polymer structure and dynamics, including intrinsically disordered peptides, protein folding, and enzyme activity, many questions remain that cannot be answered by methodology based on artificial intelligence, X-ray, or NMR spectroscopy but maybe by fluorescence spectroscopy. The theory of [...] Read more.
In the huge field of polymer structure and dynamics, including intrinsically disordered peptides, protein folding, and enzyme activity, many questions remain that cannot be answered by methodology based on artificial intelligence, X-ray, or NMR spectroscopy but maybe by fluorescence spectroscopy. The theory of Förster resonance energy transfer (FRET) describes how an optically excited fluorophore transfers its excitation energy through space to an acceptor moiety—with a rate that depends on the distance between donor and acceptor. When the donor and acceptor moiety are conjugated to different sites of a flexible peptide chain or any other linear polymer, the pair could in principle report on chain structure and dynamics, on the site-to-site distance distribution, and on the diffusion coefficient of mutual site-to-site motion of the peptide chain. However, the dependence of FRET on distance distribution and diffusion is not defined by a closed analytical expression but by a partial differential equation (PDE), by the Haas-Steinberg equation (HSE), which can only be solved by time-consuming numerical methods. As a second complication, time-resolved FRET measurements have thus far been deemed necessary. As a third complication, the evaluation requires a computationally demanding but indispensable global analysis of an extended experimental data set. These requirements have made the method accessible to only a few experts. Here, we show how the Haas-Steinberg equation leads to a closed analytical expression (CAE), the Haas-Steinberg-Jacob equation (HSJE), which relates a diffusion-diagnosing parameter, the effective donor–acceptor distance, to the augmented diffusion coefficient, J, composed of the diffusion coefficient, D, and the photophysical parameters that characterize the used FRET method. The effective donor–acceptor distance is easily retrieved either through time-resolved or steady-state fluorescence measurements. Any global fit can now be performed in seconds and minimizes the sum-of-square difference between the experimental values of the effective distance and the values obtained from the HSJE. In summary, the HSJE can give a decisive advantage in applying the speed and sensitivity of FRET spectroscopy to standing questions of polymer structure and dynamics. Full article
(This article belongs to the Special Issue Current Directions and Innovations in Fluorescence Techniques for Characterization of Polymers and Polymeric Materials)
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Review

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21 pages, 4087 KiB  
Review
Bright and Stable Nanomaterials for Imaging and Sensing
by José Paulo Sequeira Farinha
Polymers 2023, 15(19), 3935; https://doi.org/10.3390/polym15193935 - 29 Sep 2023
Viewed by 885
Abstract
This review covers strategies to prepare high-performance emissive polymer nanomaterials, combining very high brightness and photostability, to respond to the drive for better imaging quality and lower detection limits in fluorescence imaging and sensing applications. The more common approaches to obtaining high-brightness nanomaterials [...] Read more.
This review covers strategies to prepare high-performance emissive polymer nanomaterials, combining very high brightness and photostability, to respond to the drive for better imaging quality and lower detection limits in fluorescence imaging and sensing applications. The more common approaches to obtaining high-brightness nanomaterials consist of designing polymer nanomaterials carrying a large number of fluorescent dyes, either by attaching the dyes to individual polymer chains or by encapsulating the dyes in nanoparticles. In both cases, the dyes can be covalently linked to the polymer during polymerization (by using monomers functionalized with fluorescent groups), or they can be incorporated post-synthesis, using polymers with reactive groups, or encapsulating the unmodified dyes. Silica nanoparticles in particular, obtained by the condensation polymerization of silicon alcoxides, provide highly crosslinked environments that protect the dyes from photodegradation and offer excellent chemical modification flexibility. An alternative and less explored strategy is to increase the brightness of each individual dye. This can be achieved by using nanostructures that couple dyes to plasmonic nanoparticles so that the plasmon resonance can act as an electromagnetic field concentrator to increase the dye excitation efficiency and/or interact with the dye to increase its emission quantum yield. Full article
(This article belongs to the Special Issue Current Directions and Innovations in Fluorescence Techniques for Characterization of Polymers and Polymeric Materials)
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