Collective fluorescence switching of counterion-assembled dyes in polymer nanoparticles
Open accessAbstract
The current challenge in the field of fluorescent nanoparticles (NPs) for bioimaging is to achieve extreme brightness and external control of their emission using biodegradable materials. Here we propose a new concept of fluorescent polymer NPs, doped with ionic liquid-like salts of a cationic dye (octadecyl rhodamine B) with a bulky hydrophobic counterion (fluorinated tetraphenylborate) that serves as spacer minimizing dye aggregation and self-quenching. The obtained 40-nm poly(D,L-lactide-co-glycolide) NPs containing up to 500 dyes are brighter than quantum dots and exhibit photo-induced reversible on/off fluorescence switching, never reported for dye-doped NPs. We show that this collective switching of hundreds of dyes is due to ultrafast excitation energy transfer and can be used for super-resolution imaging. These NPs, being spontaneously endocytosed by living cells, feature high signal-to-noise ratio and absence of toxicity. The counterion-based concept opens the way to a new class of nanomaterials for sensing, imaging and light harvesting.
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These bulky counterions are characterized by their large size, high hydrophobicity, and strong delocalization of the negative charge over the large volume of the anion, and they can serve as spacers (or insulators) between cationic dyes.
“These bulky conterions are characterized by their large size, high hydrophobicity, and strong delocalization of the negative charge over the large volume of the anion, and they can serve as spacers (or insulators) between cationic dyes.”
From The Pursuit of Shortwave Infrared-Emitting Nanoparticles with Bright Fluorescence through Molecular Design and Excited-State Engineering of Molecular Aggregates (2022) · cites this paper as [153]
The introduction describes the counterions as bulky and hydrophobic, and the Discussion says they prevent cationic dyes from stacking, supporting the spacer analogy. The Discussion does not describe the negative charge as strongly delocalized over the anion’s volume; instead, it describes F5-TPB as having high negative charge density at its surface. The indexed passages provide section labels but no page numbers. (LLM, conf=0.88)
Experimental — accuracy not yet measuredBulky hydrophobic counterions, generally weakly coordinating anions, may serve as a spacer that minimizes dye aggregation and self-quenching.
“Bulky hydrophobic counterions, generally weakly coordinating anions (e.g., perchlorate, tetraphenylborate, tetrakis(4-fluorophenyl)borate, and tetrakis(pentafluorophenyl)), may serve as a spacer that minimizes dye aggregation and self-quenching.153”
From The Pursuit of Shortwave Infrared-Emitting Nanoparticles with Bright Fluorescence through Molecular Design and Excited-State Engineering of Molecular Aggregates (2022) · cites this paper as [153]
The Discussion (page unavailable) says bulky fluorinated organic counterions reduce dye aggregation and self-quenching, supporting the spacer concept for the tetraphenylborate analogues studied. But the Photophysics section reports that R18 perchlorate quenched rapidly at higher dye loading, while the Preparation section describes its salt as amphiphilic rather than comparably hydrophobic. The paper therefore does not support including perchlorate as an effective example. (LLM, conf=0.88)
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References 56 · Cited by 226
- Authors
- Reisch, A., Didier, P., Richert, L., Oncul, S., Arntz, Y., Mély, Y., & Klymchenko, A. S.
- Affiliations
- Centre National de la Recherche Scientifique (FR)
- Corresponding author
- Klymchenko, Andrey S.
- ORCID
- Venue
- Nature Communications
- Published
- 2014-06-09
- Volume
- 5
- Issue
- 1
- Pages
- 4089-4089
- ISSN
- 2041-1723 (ISSN-L)
- OpenAlex
- W1969927982
- Cited by
- 226
- References
- 56
- Citations by year
- 2026: 13 · 2025: 15 · 2024: 17 · 2023: 16 · 2022: 24 · 2021: 29 · 2020: 28 · 2019: 16 · 2018: 20 · 2017: 15 · 2016: 15 · 2015: 14 · 2014: 4
- FWCI
- 7.26
- Type
- journal article
- Language
- en
- Open access
- bronze
- doi.org
- Licence
- Locations
- Nature Communications (publishedVersion)
- PubMed (publishedVersion)
- HAL (submittedVersion)
- RePEc: Research Papers in Economics (submittedVersion)
- Funders
- Agence Nationale de la Recherche (ANR-11-JS07-014-01, ANR-11-JS07-0014)
- Centre National de la Recherche Scientifique
- Topics
- Physical Sciences › Materials Science › Materials Chemistry › Luminescence and Fluorescent Materials
- Physical Sciences › Materials Science › Materials Chemistry › Quantum Dots Synthesis And Properties
- Physical Sciences › Chemistry › Spectroscopy › Molecular Sensors and Ion Detection
- Keywords
- poly(lactic-co-glycolic acid), excitation energy transfer, dye aggregation, self-quenching, super-resolution imaging, bioimaging, biodegradable nanomaterials
- MeSH terms
- Fluorescent Dyes, Microscopy, Fluorescence, Polymers, Rhodamines, Tetraphenylborate, Microscopy, Atomic Force, Nanotechnology, Nanoparticles, Signal-To-Noise Ratio
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