Excimer Emission in J-Aggregates

Dimitriev, Oleg P.; Piryatinskiĭ, Yu. P.; Slominskii, Yu. L.

doi:10.1021/acs.jpclett.8b00481

Cited by 55 publications

(60 citation statements)

References 29 publications

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“…Interestingly, the GSB feature demonstrated relatively slow vibronic relaxation processes, that is, about 20–50 ps, before recombination started (Figure S2a, Supporting Information). Such a relaxation is probably due to the torsional motion of the bulky benzo[ e ]indolium groups of 1859, which is attributed to the transformation of the trans‐ to cis ‐ form in the excited single state of tricarbocyanine dyes . This assumption is consistent with the shift of the maximum emission with respect to the excitation, which demonstrates the rise time of 100–200 ps (Figure S3, Supporting Information).…”

Section: Resultssupporting

confidence: 70%

Reversible Charge Transfer with Single‐Walled Carbon Nanotubes Upon Harvesting the Low Energy Part of the Solar Spectrum

Menon

Slominskii

Joseph

et al. 2020

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Here, the ability of a novel near‐infrared dye to noncovalently self‐assemble onto the surface of single‐walled carbon nanotubes (SWCNTs) driven by charge‐transfer interactions is demonstrated. Steady‐state, Raman, and transient absorption spectroscopies corroborate the electron donating character of the near‐infrared dye when combined with SWCNTs, in the form of fluorescence quenching of the excited state of the dye, n‐doping of SWCNTs, and reversible charge transfer, respectively. Formation of the one‐electron oxidized dye as a result of interactions with SWCNTs is supported by spectroelectrochemical measurements. The ultrafast electronic process in the near‐infrared dye, once immobilized onto SWCNTs, starts with the formation of excited states, which decay to the ground state via the intermediate population of a fully charge‐separated state, with characteristic time constants for the charge separation of 1.5 ps and charge recombination of 25 ps, as derived from the multiwavelength global analysis. Of great relevance is the fact that charge‐transfer occurs from the hot excited state of the near‐infrared dye to SWCNTs.

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Section: Resultssupporting

confidence: 70%

Reversible Charge Transfer with Single‐Walled Carbon Nanotubes Upon Harvesting the Low Energy Part of the Solar Spectrum

Menon

Slominskii

Joseph

et al. 2020

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“…However,t he unusually large Stokes shift observed for the J-type nanoaggregates might be the result of the combination of excited-state Hb ondinga nd charge-transfer effects. [18] The relative population of these two forms of aggregates was found to be largely dependentont he membrane microenvironment.…”

Section: Emission Behavior Of Membrane-boundpytpy In Watermentioning

confidence: 96%

Highly Responsive Fluorescent Assemblies Allow for Unique, Multiparametric Sensing of the Phospholipid Membrane Environment

Gulyani

Dey

Bhattacharya

2018

Chemistry A European J

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Despite decades-long extensive research, probes that provide a comprehensive description of the lipid membrane microenvironment are still lacking. We report here a 'smart' pyrene-terpyridine probe for multiparametric sensing of lipid membranes; wherein the complexity of the local microenvironment can be described by distinct features of the probe fluorescence. The self-assembly of the probe molecules in phospholipid bilayers is sensitive to membrane order and phase state. The self-assembled probes show a unique emission, influenced by dye-dye interactions and excited state charge transfer. Moreover, this emission is sensitive to interfacial hydration, with very specific changes in emission wavelengths and fluorescence lifetimes as lipid compositions and properties are varied. In parallel, changes in lipid order along with hydration affect the ground state interactions in dye-aggregates and thus can be measured through ratiometric changes in excitation and emission readouts. In addition, fluorescence anisotropy measurements provide another way to study the nature of dye-aggregates in lipid bilayers. Overall, here we demonstrate how multiple aspects of membrane microenvironment can be sensed through unique fluorescence signatures of this ҆smart҆ probe in lipid membranes, and establish a new paradigm in lipid membrane sensing.

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“…These findings underscore the diverse requirements for charge and energy delocalization across p-stacked assemblies.Charge and energy dynamics across p-stacked assemblies is of critical importance in biological systems as well in the performance of functional materials. [1][2][3] Va rious p-stacked dimers capable of excimer formation and charge-resonance stabilization based upon benzene, [4][5][6][7][8] fluorene, [9][10][11][12] pyrene, [13,14] and other aromatic donors [15][16][17][18] have served as model systems to gain fundamental insight into key factors controlling charge/energy stabilization. These studies have established that the extent of the cationic charge (that is,hole) and exciton stabilization/delocalization is dependent on the orbital overlap between the chromophores,a nd is optimal when the p-stacked assembly adopts ap erfect sandwich-like arrangement, where orbital overlap and electronic coupling are at their maxima.…”

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confidence: 99%

The Role of Torsional Dynamics on Hole and Exciton Stabilization in π‐Stacked Assemblies: Design of Rigid Torsionomers of a Cofacial Bifluorene

et al. 2018

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Exciton and charge delocalization across π-stacked assemblies is of importance in biological systems and functional polymeric materials. To examine the requirements for exciton and hole stabilization, cofacial bifluorene (F2) torsionomers were designed, synthesized, and characterized: unhindered (model) F2, sterically hindered F2, and cyclophane-like F2, where fluorenes are locked in a perfect sandwich orientation via two methylene linkers. This set of bichromophores with varied torsional rigidity and orbital overlap shows that exciton stabilization requires a perfect sandwich-like arrangement, as seen by strong excimeric-like emission only in F2 and F2. In contrast, hole delocalization is less geometrically restrictive and occurs even in sterically hindered F2, as judged by 160 mV hole stabilization and a near-IR band in the spectrum of its cation radical. These findings underscore the diverse requirements for charge and energy delocalization across π-stacked assemblies.

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Excimer Emission in J-Aggregates

Cited by 55 publications

References 29 publications

Reversible Charge Transfer with Single‐Walled Carbon Nanotubes Upon Harvesting the Low Energy Part of the Solar Spectrum

Reversible Charge Transfer with Single‐Walled Carbon Nanotubes Upon Harvesting the Low Energy Part of the Solar Spectrum

Highly Responsive Fluorescent Assemblies Allow for Unique, Multiparametric Sensing of the Phospholipid Membrane Environment

The Role of Torsional Dynamics on Hole and Exciton Stabilization in π‐Stacked Assemblies: Design of Rigid Torsionomers of a Cofacial Bifluorene

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