Control of the fluorescence lifetime in dye based nanoparticles

Stenspil, Stine G.; Chen, Junsheng; Liisberg, Mikkel B.; Flood, Amar H.; Laursen, Bo W.

doi:10.1039/d3sc05496a

Cited by 4 publications

(2 citation statements)

References 33 publications

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“…This is the case for e.g. time-resolved techniques, 58,128,138 super resolution, 40 and circular polarized emission. 139 Development of dye based NPs specifically for such readouts is a promising direction.…”

Section: Future Outlookmentioning

confidence: 95%

“…This doping strategy was demonstrated for several SMILES materials showing large improvement of quantum yields and fluorescence lifetimes approaching the intrinsic molecular values and was since translated to SMILES NPs. 41,128 Introduction of dopant dyes in the NP core has been used in several NP strategies to boost the fluorescence brightness, 42,64,129–131 while introduction of acceptor dyes to the NP surface also has been used to develop sensing properties e.g. for DNA/RNA hybridization assays.…”

Section: Doping and MIX Of Strategiesmentioning

confidence: 99%

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Photophysics of fluorescent nanoparticles based on organic dyes – challenges and design principles

Stenspil,

Laursen

2024

Chem. Sci.

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Section: Future Outlookmentioning

confidence: 95%

Section: Doping and MIX Of Strategiesmentioning

confidence: 99%

Photophysics of fluorescent nanoparticles based on organic dyes – challenges and design principles

Stenspil,

Laursen

2024

Chem. Sci.

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Accelerated Computer-Aided Screening of Optical Materials: Investigating the Potential of Δ-SCF Methods to Predict Emission Maxima of Large Dye Molecules

Tripathy,

Flood,

Raghavachari

2024

J. Phys. Chem. A

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Accurate simulation of electronic excited states of large chromophores is often difficult due to the computationally expensive nature of existing methods. Common approximations such as fragmentation methods that are routinely applied to ground-state calculations of large molecules are not easily applicable to excited states due to the delocalized nature of electronic excitations in most practical chromophores. Thus, special techniques specific to excited states are needed. Δ-SCF methods are one such approximation that treats excited states in a manner analogous to that for ground-state calculations, accelerating the simulation of excited states. In this work, we employed the popular initial maximum overlap method (IMOM) to avoid the variational collapse of the electronic excited state orbitals to the ground state. We demonstrate that it is possible to obtain emission energies from the first singlet (S 1 ) excited state of many thousands of dye molecules without any external intervention. Spin correction was found to be necessary to obtain accurate excitation and emission energies. Using thousands of dye-like chromophores and various solvents (12,318 combinations), we show that the spin-corrected initial maximum overlap method accurately predicts emission maxima with a mean absolute error of only 0.27 eV. We further improved the predictive accuracy using linear fit-based corrections from individual dye classes to achieve an impressive performance of 0.17 eV. Additionally, we demonstrate that IMOM spin density can be used to identify the dye class of chromophores, enabling improved prediction accuracy for complex dye molecules, such as dyads (chromophores containing moieties from two different dye classes). Finally, the convergence behavior of IMOM excited state SCF calculations is analyzed briefly to identify the chemical space, where IMOM is more likely to fail.

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Fluorophore multimerization on a PEG backbone as a concept for signal amplification and lifetime modulation

Reiber,

Hübner,

Dose

et al. 2024

Sci Rep

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Fluorescent labels have strongly contributed to many advancements in bioanalysis, molecular biology, molecular imaging, and medical diagnostics. Despite a large toolbox of molecular and nanoscale fluorophores to choose from, there is still a need for brighter labels, e.g., for flow cytometry and fluorescence microscopy, that are preferably of molecular nature. This requires versatile concepts for fluorophore multimerization, which involves the shielding of dyes from other chromophores and possible quenchers in their neighborhood. In addition, to increase the number of readout parameters for fluorescence microscopy and eventually also flow cytometry, control and tuning of the labels’ fluorescence lifetimes is desired. Searching for bright multi-chromophoric or multimeric labels, we developed PEGylated dyes bearing functional groups for their bioconjugation and explored their spectroscopic properties and photostability in comparison to those of the respective monomeric dyes for two exemplarily chosen fluorophores excitable at 488 nm. Subsequently, these dyes were conjugated with anti-CD4 and anti-CD8 immunoglobulins to obtain fluorescent conjugates suitable for the labeling of cells and beads. Finally, the suitability of these novel labels for fluorescence lifetime imaging and target discrimination based upon lifetime measurements was assessed. Based upon the results of our spectroscopic studies including measurements of fluorescence quantum yields (QY) and fluorescence decay kinetics we could demonstrate the absence of significant dye-dye interactions and self-quenching in these multimeric labels. Moreover, in a first fluorescence lifetime imaging (FLIM) study, we could show the future potential of this multimerization concept for lifetime discrimination and multiplexing.

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Control of the fluorescence lifetime in dye based nanoparticles

Abstract: Fluorescent dye based nanoparticles (NPs) have received increased interest due to their high brightness and stability. In fluorescence microscopy and assays, high signal to background ratios and multiple channels of...

Cited by 4 publications

References 33 publications

Photophysics of fluorescent nanoparticles based on organic dyes – challenges and design principles

Photophysics of fluorescent nanoparticles based on organic dyes – challenges and design principles

Accelerated Computer-Aided Screening of Optical Materials: Investigating the Potential of Δ-SCF Methods to Predict Emission Maxima of Large Dye Molecules

Fluorophore multimerization on a PEG backbone as a concept for signal amplification and lifetime modulation

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