Evidence of Exciton Self-Trapping in Pseudoisocyanine J-Aggregates Formed in Layered Polymer Films

Sorokin, A. V.; Pereverzev, Nikita V.; Grankina, Irina I.; Yefimova, Svetlana; Malyukin, Yu. V.

doi:10.1021/acs.jpcc.5b09940

Cited by 40 publications

(92 citation statements)

References 56 publications

(197 reference statements)

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“…This theoretical investigation is motivated by several studies that have noted deviations from Förster theory's characteristic − R 6 dependence on the rate of EET (the rate of EET is proportional to the square of the coupling) [41][42][43]. Any deviations from Förster theory could have an impact on design strategies for the development of mesoscopic energy harvesting materials [47][48][49][50][51][52][53][54][55][56][57][58][59].…”

Section: Resultsmentioning

confidence: 99%

A quantum dynamical comparison of the electronic couplings derived from quantum electrodynamics and Förster theory: application to 2D molecular aggregates

Frost

Jones

2014

New J. Phys.

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The objective of this study is to investigate under what circumstances Förster theory of electronic (resonance) energy transfer breaks down in molecular aggregates. This is achieved by simulating the dynamics of exciton diffusion, on the femtosecond timescale, in molecular aggregates using the Liouville-von Neumann equation of motion. Specifically the focus of this work is the investigation of both spatial and temporal deviations between exciton dynamics driven by electronic couplings calculated from Förster theory and those calculated from quantum electrodynamics. The quantum electrodynamics (QED) derived couplings contain medium-and far-zone terms that do not exist in Förster theory. The results of the simulations indicate that Förster coupling is valid when the dipole centres are within a few nanometres of one another. However, as the distance between the dipole centres increases from 2 nm to 10 nm, the intermediate-and far-zone coupling terms play non-negligible roles and Förster theory begins to break down. Interestingly, the simulations illustrate how contributions to the exciton dynamics from the intermediate-and far-zone coupling terms of QED are quickly washed-out by the near-zone mechanism of Förster theory for lattices comprising closely packed molecules. On the other hand, in the case of sparsely packed arrays, the exciton dynamics resulting from the different theories diverge within the 100 fs lifetime of the trajectories. These results could have implications for the application of spectroscopic ruler techniques as well as design principles relating to energy harvesting materials.

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Section: Resultsmentioning

confidence: 99%

A quantum dynamical comparison of the electronic couplings derived from quantum electrodynamics and Förster theory: application to 2D molecular aggregates

Frost

Jones

2014

New J. Phys.

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“…[43] On the other hand, such disorder can also induce exciton self-trapping. [44] We note that both the almost linear PL intensity as a function of excitation fluence in lamellar films as well as the sub-linear behavior in platelets remained constant (in the error range for the exponent of ±0.05) within the temperature range of the measurements (Figure S9, Supporting Information). This suggests a temperature-independent charge generation and trapping rate and a minor role of temperature-driven exciton or charge diffusion for this kind of quenching process.…”

Section: Exciton Dynamics In Platelets and Lamellar Films At Low Tempmentioning

confidence: 77%

Exciton Dynamics and Effects of Structural Order in Morphology‐Controlled J‐Aggregate Assemblies

Anantharaman

Stöferle

Nüesch

et al. 2018

Adv Funct Materials

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Narrow-band photoluminescence (PL) together with high quantum efficiency from organic molecules is essential for high color purity emitters. Supramolecular assemblies like Jaggregates are promising materials due to their narrow PL signal with full-width at half maximum (FWHM) < 20 nm. However, their micro-crystalline nature and coherent exciton migration results in strong non-radiative exciton recombination at the grain boundaries that diminish the photoluminescence quantum yield (PLQY), and possibilities for improving the crystallinity by tuning the growth mechanism were limited. Here, we demonstrate two distinct routes to grow different J-aggregate morphologies like platelets and lamellar crystals with Received: ((will be filled in by the editorial staff))Revised: ((will be filled in by the editorial staff))

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“…Based on the intensity increase by cooling, they claimed that the long-wavelength FL originates from the trapping states lying below the exciton states that are populated by the energy transfer from the excitons. Sorokin et al reported that PIC J-aggregates in layered films of poly(sodium 4-styrenesulfonate) showed a broad FL band peaking at λ = 618 nm at T = 77 K. The authors assigned this FL to the emission from self-trapping exciton states, with the support of time-resolved FL spectroscopy measurements …”

Section: Resultsmentioning

confidence: 94%

“…Since the PIC J-aggregates embedded in polymer films are stable and resistant to photobleaching, these samples are well-suited for spectroscopic investigations. However, the optical properties of the J-aggregates in these samples differ considerably depending on the polymers used, as well as on the film fabrication methods, indicating that the interaction between the aggregates and the surrounding polymers strongly influences their optical properties. − This may hinder the investigation of the intrinsic optical properties of J-aggregates. Moreover, the polymers that surround the J-aggregates prevent a direct measurement of their geometry, for example, using an atomic force microscope.…”

Section: Introductionmentioning

confidence: 99%

Fabrication and Optical Properties of Fiber-Shaped Pseudoisocyanine J-Aggregates Grown Directly on a Glass Substrate

2021

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We developed a novel method for the direct growth of fiber-shaped J-aggregates of pseudoisocyanine chloride (PIC-Cl) on a glass substrate via solution-phase self-assembly. A network of J-aggregate fibers that homogeneously covered the entire surface area of the substrate with dimensions of 22 mm × 22 mm was formed. Moreover, the width of the fibers can be controlled over a wide range (100 nm−5 μm) by changing the solution concentration. We found that the fibers prepared using this method were nearly endless. The formation mechanism of the endless fibers was discussed in terms of end-cap energy. We performed spectroscopic investigations on the samples and found that their optical properties were strongly fiber-width-dependent. On the basis of the spectral analysis and the results from low-temperature fluorescence spectroscopy, we propose that the fiberwidth-dependence can be attributed to a difference in the density of disorder created in the fibers.

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Evidence of Exciton Self-Trapping in Pseudoisocyanine J-Aggregates Formed in Layered Polymer Films

Cited by 40 publications

References 56 publications

A quantum dynamical comparison of the electronic couplings derived from quantum electrodynamics and Förster theory: application to 2D molecular aggregates

A quantum dynamical comparison of the electronic couplings derived from quantum electrodynamics and Förster theory: application to 2D molecular aggregates

Exciton Dynamics and Effects of Structural Order in Morphology‐Controlled J‐Aggregate Assemblies

Fabrication and Optical Properties of Fiber-Shaped Pseudoisocyanine J-Aggregates Grown Directly on a Glass Substrate

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