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Review
. 2021 Dec 15;13(24):4404.
doi: 10.3390/polym13244404.

Chromophoric Dendrimer-Based Materials: An Overview of Holistic-Integrated Molecular Systems for Fluorescence Resonance Energy Transfer (FRET) Phenomenon

Sebastián Bonardd  1   2 , David Díaz Díaz  1   2   3 , Angel Leiva  4 , César Saldías  4
Affiliations
Review

Chromophoric Dendrimer-Based Materials: An Overview of Holistic-Integrated Molecular Systems for Fluorescence Resonance Energy Transfer (FRET) Phenomenon

Sebastián Bonardd et al. Polymers (Basel). .

Abstract

Dendrimers (from the Greek dendros → tree; meros → part) are macromolecules with well-defined three-dimensional and tree-like structures. Remarkably, this hyperbranched architecture is one of the most ubiquitous, prolific, and recognizable natural patterns observed in nature. The rational design and the synthesis of highly functionalized architectures have been motivated by the need to mimic synthetic and natural-light-induced energy processes. Dendrimers offer an attractive material scaffold to generate innovative, technological, and functional materials because they provide a high amount of peripherally functional groups and void nanoreservoirs. Therefore, dendrimers emerge as excellent candidates since they can play a highly relevant role as unimolecular reactors at the nanoscale, acting as versatile and sophisticated entities. In particular, they can play a key role in the properties of light-energy harvesting and non-radiative energy transfer, allowing them to function as a whole unit. Remarkably, it is possible to promote the occurrence of the FRET phenomenon to concentrate the absorbed energy in photoactive centers. Finally, we think an in-depth understanding of this mechanism allows for diverse and prolific technological applications, such as imaging, biomedical therapy, and the conversion and storage of light energy, among others.

Keywords: FRET; chromophoric dendrimers; holistic molecular systems.

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Conflict of interest statement

The authors declare no conflict of interest.

Figures

Figure 1
Figure 1
Representative illustration of the general structure of dendrimers. Reprinted with permission from [32]. Copyright 2010 Elsevier.
Figure 2
Figure 2
The holistic approach of hierarchical levels of organization of biological models across temporal and spatial scales. Reprinted with permission from reference [47]. Copyright 2017 Frontiers Media.
Figure 3
Figure 3
Representative structure of the cell showing their constituent organelles. Reprinted with permission from reference [50]. Copyright 2020 Springer.
Figure 4
Figure 4
Illustration of two entangled photons. The state of one of them is instantaneously transferred to the other one. Reprinted with permission from [51]. Copyright 2015 Serials Publications.
Figure 5
Figure 5
Dendrimer-based systems act as materials for (a) photocurrent generation, (b) sensor food spoilage detection, (c) semiconducting devices, and (d) enhancing the power conversion efficiency of solar cells. Reprinted with permission from [58] Copyright 2019 Springer; [59] Copyright 2021 American Chemical Society; [60] Copyright 2020 Royal Society of Chemistry; [61] Copyright 2021 Springer.
Figure 5
Figure 5
Dendrimer-based systems act as materials for (a) photocurrent generation, (b) sensor food spoilage detection, (c) semiconducting devices, and (d) enhancing the power conversion efficiency of solar cells. Reprinted with permission from [58] Copyright 2019 Springer; [59] Copyright 2021 American Chemical Society; [60] Copyright 2020 Royal Society of Chemistry; [61] Copyright 2021 Springer.
Figure 6
Figure 6
(a) Description of the FRET mechanism. D (A) and D* (A*) are the ground state and excited state of the donor unit (acceptor unit), respectively; h is the Planck’s constant; ν is the frequency of the radiation. (b) Representation of the FRET phenomenon by Jablonsky diagrams. The excited state of the donor unit (spatially close to the acceptor unit) reaches relaxation by the FRET mechanism exciting the acceptor (non-radiative energy transfer). The relaxation stage of the acceptor unit is evidenced by the fluorescence process emitting light. Note that the emitted light is a lower wavelength than the emission of the donor in a regular fluorescence process. Reprinted with permission from [92]. Copyright 2016 SAGE Publications.
Figure 7
Figure 7
The density of states obtained from the spectral overlap between donor-emission (Em.) and acceptor-excitation (Ex.) bands. The efficiency of the FRET phenomenon is maximizedwhen the donor and acceptor molecules are at an average distance of 10 nm from each other, and their respective dipole moments are oriented in parallel. Reprinted with permission from [101]. Copyright 2017 Elsevier.
Figure 8
Figure 8
Representation of FRET efficiencies between chromophores using, as an initial donor, coumarin (blue), an intermediate fluorol (green), and a final acceptor perylene (red). Reprinted with permission from [135]. Copyright 2002 Royal Society of Chemistry.
Figure 9
Figure 9
(a) Illustration of the energetically minimized structure of the triad constituting naphthalenemonoimide(blue), perylenemonoimide(green), and terrylenediimide(red) moieties. (b) Center-to-center interchromophoric distances calculated from the energetically minimized structure. Reprinted with permission from [143]. Copyright 2005 American Chemical Society.
Figure 10
Figure 10
Mechanism of singlet oxygen photosensitization via indirect excitation of the photosensitizer (porphyrin) by two-photon-excited FRET from distanced chromophores present into a dendrimer. Reprinted with permission from [149]. Copyright 2005 American Chemical Society.
Figure 11
Figure 11
(a) Averaged values of the overall trajectories of non-adiabatic coupling vector of S2→S1 hop and (b) illustration of the effective hop process in the dendron at ≈ 5 fs. Reprinted with permission from [155]. Copyright 2009 American Chemical Society.
Figure 12
Figure 12
(a) Chemical structure of first-generation pyrene dendronized porphyrins having a metal center and (b) absolute emission spectra recorded in THF for the metal-free (black line) and metalated porphyrins (M = Zn and Mg are represented by red and blue lines, respectively). Reprinted with permission from [166]. Copyright 2021 Elsevier.
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