Template-free H-dimer and H-aggregate formation by dimeric carbocyanine dyes

Patlolla, Prathap Reddy; Mahapatra, Amarjyoti Das; Mallajosyula, Sairam S.; Datta, Bhaskar

doi:10.1039/c8nj00371h

Cited by 11 publications

(5 citation statements)

References 32 publications

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“…Other aggregates, including H-aggregates and J-aggregates, can also form . H-aggregates are characterized by cofacial stacking between the monomeric units that results in hypsochromic shifts (or H-shifts) in the absorption spectra relative to the monomeric species . J-aggregates, in contrast, are slipped-stack arrangements of monomeric units that have bathochromic shifts in their absorption spectra and increased extinction coefficients in those bathochromically shifted bands …”

Section: Underlying Principles Of Chemosensorsmentioning

confidence: 99%

“…317 H-aggregates are characterized by cofacial stacking between the monomeric units that results in hypsochromic shifts (or H-shifts) in the absorption spectra relative to the monomeric species. 318 J-aggregates, in contrast, are slippedstack arrangements of monomeric units that have bathochromic shifts in their absorption spectra and increased extinction coefficients in those bathochromically shifted bands. 319 The molecular orientation between the donor and acceptor can have profound effects on the efficiency of energy transfer processes, with the effects intimately dependent on the particular energy transfer mechanism.…”

Section: Mechanisms Of Fluorescencementioning

confidence: 99%

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Supramolecular Luminescent Sensors

2018

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There is great need for stand-alone luminescence-based chemosensors that exemplify selectivity, sensitivity, and applicability and that overcome the challenges that arise from complex, real-world media. Discussed herein are recent developments toward these goals in the field of supramolecular luminescent chemosensors, including macrocycles, polymers, and nanomaterials. Specific focus is placed on the development of new macrocycle hosts since 2010, coupled with considerations of the underlying principles of supramolecular chemistry as well as analytes of interest and common luminophores. State-of-the-art developments in the fields of polymer and nanomaterial sensors are also examined, and some remaining unsolved challenges in the area of chemosensors are discussed. CONTENTS 4.4. Explosives 4.5. Pharmaceutical Agents 4.6. Biologically Relevant 4.6.1. Adenosine Triphosphate (ATP)

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Section: Underlying Principles Of Chemosensorsmentioning

confidence: 99%

Section: Mechanisms Of Fluorescencementioning

confidence: 99%

Supramolecular Luminescent Sensors

2018

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“…Conversely, both compounds appear to experience an increase in intensity of a higher-energy shoulder when placed in a predominantly aqueous environment ( C8S3- p -Br shown in Figure S9). Since the absorption bands of trimethine cyanine dye H-aggregates are characterized by exhibiting similar hypsochromic shifts, − it is possible that this change in spectral shape is the result of H-type aggregation. Clearly, both the presence and attachment position of halogen atoms on this cyanine dye system play an important role in controlling aggregation.…”

Section: Results and Discussionmentioning

confidence: 99%

Synthetic Access to Benzimidacarbocyanine Dyes to Tailor Their Aggregation Properties

et al. 2021

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Developing structure−aggregation relationships of cyanine dyes is crucial for controlling their optical properties for various uses. This study develops a synthetic route and the structure-dependent self-assembly of a family of benzimidacarbocyanine dyes for J-or H-aggregation properties. It was found that both the presence and placement of halogen atoms play a defining role in the resulting supramolecular interactions of these compounds.

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“…The coupling Ω between molecules can either have a dipolar or a different origin, see SI. Typical H-dimers feature splittings between their bright and dark states of several k B T , and the lower state may be many hundreds times less bright than the upper state [24][25][26][27].…”

Section: Fig 1 (A)mentioning

confidence: 99%

“…Many molecular aggregates, both naturally occurring as well as artificially synthesized, display bright and dark states in their single-excitation manifold [24][25][26][27]: J-aggregates are characterized by a bright state below the energy of the monomer absorption peak, while Haggregates are characterized by a bright state above the energy of the monomer absorption peak. Cooperative properties, such as those seen in photosynthetic aggregates, have inspired many proposals for engineering artificial light-harvesting devices [28][29][30][31][32][33][34][35].…”

Section: Introductionmentioning

confidence: 99%

Bio-inspired natural sunlight-pumped lasers

et al. 2021

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Even though sunlight is by far the most abundant renewable energy source available to humanity, its dilute and variable nature has kept efficient ways to collect, store, and distribute this energy tantalisingly out of reach. Turning the incoherent energy supply provided by the Sun into a coherent laser beam would overcome several of the practical limitations inherent in using sunlight as a source of clean energy: laser beams travel nearly losslessly over large distances, and they are effective at driving chemical reactions which convert sunlight into chemical energy. Here we propose a bio-inspired blueprint for a novel type of laser with the aim of upgrading unconcentrated natural sunlight into a coherent laser beam. Our proposed design constitutes an improvement of several orders of magnitude over existing comparable technologies: state-of-the-art solar pumped lasers operate above 1000 suns (corresponding to 1000 times the natural sunlight power). In order to achieve lasing with the extremely dilute power provided by natural sunlight, we here propose a laser medium comprised of molecular aggregates inspired by the architecture of natural photosynthetic complexes. Such complexes, by exploiting a highly symmetric arrangement of molecules organized in a hierarchy of energy scales, exhibit a very large internal efficiency in harvesting photons from a power source as dilute as natural sunlight. Specifically, we consider substituting the reaction center of photosynthetic complexes in purple bacteria (Rhodobacter Sphaeroides) with a suitably engineered molecular dimer composed of two strongly coupled chromophores. We show that if pumped by the surrounding photosynthetic complex, which efficiently collects and concentrates solar energy, the core dimer structure can reach population inversion, and reach the lasing threshold under natural sunlight. The design principles proposed here will also pave the way for developing other bio-inspired quantum devices.

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Template-free H-dimer and H-aggregate formation by dimeric carbocyanine dyes

Abstract: Dimeric cyanine dyes self-assemble into H-dimers and H-aggregates, which experience de-aggregation with specific biomolecules.

Cited by 11 publications

References 32 publications

Supramolecular Luminescent Sensors

Supramolecular Luminescent Sensors

Synthetic Access to Benzimidacarbocyanine Dyes to Tailor Their Aggregation Properties

Bio-inspired natural sunlight-pumped lasers

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