Lévy Defects in Matrix-Immobilized J Aggregates: Tracing Intra-and Intersegmental Exciton Relaxation

Lüer, Larry; Rajendran, Sai Kiran; Stoll, Tatjana; Ganzer, Lucia; Réhault, Julien; Coles, David M.; Lidzey, David G.; Virgili, Tersilla; Cerullo, Giulio

doi:10.1021/acs.jpclett.6b02704

Cited by 11 publications

(6 citation statements)

References 40 publications

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“…However, if l 0 is expanded to several miles (without changing σ), one would experience a very smooth ride, likely never encountering a pothole. Recently, Levy distributions, non-Gaussian distributions of site-disorder that increase the occurrence of deep traps, have gained favor in describing molecular aggregate photophysics. − In addition, disorder has also been extended to the electronic couplings as well, i.e., off-diagonal disorder …”

Section: Absorption and Photoluminescence In Vibronically Coupled H- ...mentioning

confidence: 99%

Expanded Theory of H- and J-Molecular Aggregates: The Effects of Vibronic Coupling and Intermolecular Charge Transfer

2018

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The electronic excited states of molecular aggregates and their photophysical signatures have long fascinated spectroscopists and theoreticians alike since the advent of Frenkel exciton theory almost 90 years ago. The influence of molecular packing on basic optical probes like absorption and photoluminescence was originally worked out by Kasha for aggregates dominated by Coulombic intermolecular interactions, eventually leading to the classification of J- and H-aggregates. This review outlines advances made in understanding the relationship between aggregate structure and photophysics when vibronic coupling and intermolecular charge transfer are incorporated. An assortment of packing geometries is considered from the humble molecular dimer to more exotic structures including linear and bent aggregates, two-dimensional herringbone and "HJ" aggregates, and chiral aggregates. The interplay between long-range Coulomb coupling and short-range charge-transfer-mediated coupling strongly depends on the aggregate architecture leading to a wide array of photophysical behaviors.

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Section: Absorption and Photoluminescence In Vibronically Coupled H- ...mentioning

confidence: 99%

Expanded Theory of H- and J-Molecular Aggregates: The Effects of Vibronic Coupling and Intermolecular Charge Transfer

2018

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“…Understanding this vibrational structure of the absorption and PL spectra has been a key approach to explain structure-property relations. Any distortion on the vibronic progression upon aggregation helps predict the effect on the spectral features due to disorder, temperature and molecular assembling [88][89][90][91][92][93] .…”

Section: Linear Optical Signatures Of Excitons In Photophysical Aggre...mentioning

confidence: 99%

Multidimensional coherent spectroscopy of excitons in $π$-conjugated polymers

Gutiérrez-Meza¹,

Vega-Flick²,

Bittner³

et al. 2022

Preprint

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The photophysics of π-conjugated polymers has been of considerable interest over the last three decades because of their organic semiconductor properties. Primary photoexcitations, Frenkel excitons, can be probed optically by means of numerous linear spectroscopies, providing a wealth of information on the the strength of excitonic coupling, the exciton coherence length, and on the nature of the disordered energy landscape. Nonetheless, there are intrinsic limitations in the information that can be obtained with linear spectroscopy compared to non-linear coherent techniques. Examples of this are the separation of homogeneous and inhomogeneous broadening contributions to the total exciton spectral lineshape, the detailed spectral structure of exciton-vibrational coupling, and correlations between optical excitations, including exciton-charge and exciton-exciton correlations. In the present work, we discuss the role of two-dimensional coherent excitation spectroscopy and review its applications towards unravelling the basic photophysics of π-conjugated polymers as well as polymer:fullerene blends, and we argue that these techniques are now valuable mainstream materials optical probes.

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“…For instance, matrix immobilization of Jaggregates has shown Lévy (non-Gaussian) type of disorder in the films. [42] Such Lévy-type of defects are reported to significantly funnel excitons to trap states present in the film. [43] On the other hand, such disorder can also induce exciton self-trapping.…”

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

confidence: 99%

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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Lévy Defects in Matrix-Immobilized J Aggregates: Tracing Intra-and Intersegmental Exciton Relaxation

Cited by 11 publications

References 40 publications

Expanded Theory of H- and J-Molecular Aggregates: The Effects of Vibronic Coupling and Intermolecular Charge Transfer

Expanded Theory of H- and J-Molecular Aggregates: The Effects of Vibronic Coupling and Intermolecular Charge Transfer

Multidimensional coherent spectroscopy of excitons in $π$-conjugated polymers

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

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