Förster Energy Transfer in Core–Shell Nanoparticles: Theoretical Model and Monte Carlo Study

Synak, Anna; Kułak, Leszek; Bojarski, Piotr; Schlichtholz, Agnieszka

doi:10.1021/acs.jpcc.1c05314

Cited by 4 publications

(14 citation statements)

References 48 publications

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“…Energy transfer parameters used in Monte Carlo simulations were determined from the spectroscopic measurements (absorption and fluorescence spectra, donor fluorescence lifetime) performed by us (donor fluorescence quantum yield

= 3.82 ns, critical distances:

) and were fixed during the simulation process. However, for the D TR A structure, as revealed in Figure 5 b, one observes nonexponential and generally faster fluorescence intensity decay, which is a result of efficient direct energy transfer from the donor to closely located acceptors (no energy migration).This time experimental data could be very well described not only by Monte-Carlo simulations but also by Equation (2) resulting from the analytical model for N D / N A = 1/335 [ 24 ].…”

Section: Resultsmentioning

confidence: 94%

“…In the case of the D MIG A arrangement ( Figure 5 a), where one deals virtually only with donors, the observed fluorescence intensity decay is practically monoexponential with the lifetime τ = 3.82 ns. This is quite typical of systems in which energy migration is a dominant or exclusive process [ 24 , 35 , 36 , 37 ]. The experimental data obtained remain in excellent agreement with those of Monte Carlo simulations.…”

Section: Resultsmentioning

confidence: 99%

“…Monte Carlo simulations were carried out based on the aforementioned energy transfer parameters describing the considered donor (R110)–acceptor (R101) assembly. The Förster radius attains

= 5 nm while the average value of the orientation factor considered κ 2 = 0.476 (static case), as discussed in [ 24 ]. As already mentioned, the Monte Carlo data shown in Figure 5 b was obtained based on the extended model, taking into account the size variation of core-shell nanoparticles.…”

Section: Resultsmentioning

confidence: 99%

“…As already mentioned, the Monte Carlo data shown in Figure 5 b was obtained based on the extended model, taking into account the size variation of core-shell nanoparticles. Details regarding the application of the Gaussian function to comprise core-shell nanoparticles radii while modelling electronic excitation energy transfer are discussed elsewhere [ 24 ]. The formula expressed by Equation (2) was used to find the least squares best fit of the theoretical curve with experimental data for the donor fluorescence intensity decay.…”

Section: Resultsmentioning

confidence: 99%

“…Recently, we presented the theoretical model of FRET valid for single step energy transfers taking into account the size distribution of core-shell nanoparticles [ 24 ]. The coherence of the model was positively tested by the Monte-Carlo method, but until now, no experimental verification has been proposed.…”

Section: Introductionmentioning

confidence: 99%

See 4 more Smart Citations

New Core-Shell Nanostructures for FRET Studies: Synthesis, Characterization, and Quantitative Analysis

Synak

Adamska

Kułak

et al. 2022

IJMS

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This work describes the synthesis and characterization of new core-shell material designed for Förster resonance energy transfer (FRET) studies. Synthesis, structural and optical properties of core-shell nanostructures with a large number of two kinds of fluorophores bound to the shell are presented. As fluorophores, strongly fluorescent rhodamine 101 and rhodamine 110 chloride were selected. The dyes exhibit significant spectral overlap between acceptor absorption and donor emission spectra, which enables effective FRET. Core-shell nanoparticles strongly differing in the ratio of donors to acceptor numbers were prepared. This leads to two different interesting cases: typical single-step FRET or multistep energy migration preceding FRET. The single-step FRET model that was designed and presented by some of us recently for core-shell nanoparticles is herein experimentally verified. Very good agreement between the analytical expression for donor fluorescence intensity decay and experimental data was obtained, which confirmed the correctness of the model. Multistep energy migration between donors preceding the final transfer to the acceptor can also be successfully described. In this case, however, experimental data are compared with the results of Monte Carlo simulations, as there is no respective analytical expression. Excellent agreement in this more general case evidences the usefulness of this numerical method in the design and prediction of the properties of the synthesized core-shell nanoparticles labelled with multiple and chemically different fluorophores.

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= 3.82 ns, critical distances:

Section: Resultsmentioning

confidence: 94%

Section: Resultsmentioning

confidence: 99%

“…Monte Carlo simulations were carried out based on the aforementioned energy transfer parameters describing the considered donor (R110)–acceptor (R101) assembly. The Förster radius attains

Section: Resultsmentioning

confidence: 99%

Section: Resultsmentioning

confidence: 99%

Section: Introductionmentioning

confidence: 99%

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New Core-Shell Nanostructures for FRET Studies: Synthesis, Characterization, and Quantitative Analysis

Synak

Adamska

Kułak

et al. 2022

IJMS

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Nonradiative Energy Migration in Spherical Nanoparticles: Theoretical Model and Monte Carlo Study

2022

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Analytical model of nonradiative energy migration (homotransfer) within the set of chemically identical fluorophores distributed on the surface of a spherical nanoparticle is for the first time presented. The expression for emission anisotropy decay is obtained. The method of Green’s function was used to solve the master equation describing this stochastic process. An expansion in powers of the fluorophore density to investigate this finite volume problem was employed. A very good result for the Green function directly related to emission anisotropy was obtained by using the Padé approximant. It was found that emission anisotropy decay depends strongly not only on the number of fluorophores linked to the spherical nanoparticles but also on the ratio of critical radius to nanoparticle radius, which is crucial for the optimal design of antenna-like nanostructures. Coherence of the model was verified by Monte Carlo simulations and excellent quantitative agreement was found between theoretical and Monte Carlo simulation results.

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Quantitative Comparison of Recombination Rates of Core/Shell Quantum Dots in Colloidal Solutions and Self-Assembled Monolayer Superlattices

Brinn,

Yan,

Abbas

et al. 2024

J. Phys. Chem. C

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Understanding the fundamental excited-state dynamics of quantum dot thin films is key to rationally engineering high quality devices. However, studying the radiative and nonradiative recombination rates of quantum dot thin films is challenging due to the small quantity of quantum dots in a thin film. In this work, we measure the photoluminescence quantum yield of self-assembled quantum dot monolayer thin films and quantify their radiative and nonradiative rates. The recombination rates of core/shell quantum dot self-assembled monolayer superlattices are systematically compared with their colloidal solution counterparts. Both the radiative and nonradiative rates of these quantum dots were found to be enhanced in the thin film samples. The increase in the overall nonradiative rate is expected and can be attributed to the stripping of ligands from the nanocrystal surface as well as energy transfer in close-packed solid-state samples. In contrast, the increase in overall radiative rate in the film reveals a change in the fundamental optical properties of quantum dot films, suggesting that the oscillator strength of the nanocrystals increases in the films compared with in solutions. The increase in the oscillator strength is likely due to changes in the organic ligand shell coverage and its effect on the electronic band structure of the quantum dot.

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Förster Energy Transfer in Core–Shell Nanoparticles: Theoretical Model and Monte Carlo Study

Cited by 4 publications

References 48 publications

New Core-Shell Nanostructures for FRET Studies: Synthesis, Characterization, and Quantitative Analysis

New Core-Shell Nanostructures for FRET Studies: Synthesis, Characterization, and Quantitative Analysis

Nonradiative Energy Migration in Spherical Nanoparticles: Theoretical Model and Monte Carlo Study

Quantitative Comparison of Recombination Rates of Core/Shell Quantum Dots in Colloidal Solutions and Self-Assembled Monolayer Superlattices

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