Remarks on Exciton—Phonon Coupling and Exciton Transport

Munn, R. W.; Silbey, R.

doi:10.1080/00268948008069822

Cited by 34 publications

(7 citation statements)

References 22 publications

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“…Modeling EET dynamics in the intermediate coupling regime, in which the electronic coupling is comparable to the bath organization energy, is a challenging problem. This is evident in treatments of exciton migration in molecular crystals (65)(66)(67). It is becoming clear that in many photosynthetic systems, a small parameter does not exist, and a theory applicable to the intermediate coupling regime is required (8, 68-71).…”

Section: Intermediate Coupling Regimementioning

confidence: 99%

Dynamics of Light Harvesting in Photosynthesis

Cheng

Fleming

2009

Annu. Rev. Phys. Chem.

755

847

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We review recent theoretical and experimental advances in the elucidation of the dynamics of light harvesting in photosynthesis, focusing on recent theoretical developments in structure-based modeling of electronic excitations in photosynthetic complexes and critically examining theoretical models for excitation energy transfer. We then briefly describe two-dimensional electronic spectroscopy and its application to the study of photosynthetic complexes, in particular the Fenna-Matthews-Olson complex from green sulfur bacteria. This review emphasizes recent experimental observations of long-lasting quantum coherence in photosynthetic systems and the implications of quantum coherence in natural photosynthesis.

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Section: Intermediate Coupling Regimementioning

confidence: 99%

Dynamics of Light Harvesting in Photosynthesis

Cheng

Fleming

2009

Annu. Rev. Phys. Chem.

755

847

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“…In an excitonic semiconductor, two limiting cases of transport are often distinguished. 1,17 In hopping transport, the Frenkel exciton is almost localized, and they can transfer from one site to another. In molecular crystals where hopping is the main mechanism of diffusion, it is known from the Smoluchowski− Einstein theory of random walks that 18−21…”

Section: T H Imentioning

confidence: 99%

“…Detail derivation of the memory function gives the following expression in one dimension relating macroscopic EEA rate coefficient C EEA to the microscopic EEA rate and diffusion coefficient. We have already derived that B ∝ 1/τ X , therefore In an excitonic semiconductor, two limiting cases of transport are often distinguished. , In hopping transport, the Frenkel exciton is almost localized, and they can transfer from one site to another. In molecular crystals where hopping is the main mechanism of diffusion, it is known from the Smoluchowski–Einstein theory of random walks that − Therefore, from eq , for hopping-dominated diffusion, we get .…”

mentioning

confidence: 99%

Universal Inverse Scaling of Exciton–Exciton Annihilation Coefficient with Exciton Lifetime

2020

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Be it for essential everyday applications such as bright light-emitting devices or to achieve Bose−Einstein condensation, materials in which high densities of excitons recombine radiatively are crucially important. However, in all excitonic materials, exciton−exciton annihilation (EEA) becomes the dominant loss mechanism at high densities. Typically, a macroscopic parameter named EEA coefficient (C EEA ) is used to compare EEA rates between materials at the same density; higher C EEA implies higher EEA rate. Here, we find that the reported values of C EEA for 140 different materials is inversely related to the single-exciton lifetime. Since during EEA one exciton must relax to ground state, C EEA is proportional to the single-exciton recombination rate. This leads to the counterintuitive observation that the exciton density at which EEA starts to dominate is higher in a material with larger C EEA . These results broaden our understanding of EEA across different material systems and provide a vantage point for future excitonic materials and devices.

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“…RET in organic crystals, thin films, and aggregates is an area of significant current interest due to the potential application for organic optoelectronic and energy devices. Historically, this is the field where general theoretical frameworks were laid out for CRET and the effects of quantum coherence were scrutinized intensively 6,30,121,148. An important issue that dominated the literature in the 1960s to 1980s is the temperature‐dependent transition from coherent to incoherent mechanisms of the exciton mobility in molecular crystals.…”

Section: Applicationsmentioning

confidence: 99%

Resonance energy flow dynamics of coherently delocalized excitons in biological and macromolecular systems: Recent theoretical advances and open issues

Jang

Cheng

2012

WIREs Comput Mol Sci

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Recent experimental and theoretical studies suggest that biological photosynthetic complexes utilize the quantum coherence in a positive manner for efficient and robust flow of electronic excitation energy. Clear and quantitative understanding of such suggestion is important for identifying the design principles behind efficient flow of excitons coherently delocalized over multiple chromophores in condensed environments. Adaptation of such principles for synthetic macromolecular systems has also significant implication for the development of novel photovoltaic systems. Advanced theories of resonance energy transfer are presented, which can address these issues. Applications to photosynthetic light harvesting complex systems and organic materials demonstrate the capabilities of new theoretical approaches and future challenges. C 2012 John Wiley & Sons, Ltd.

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Remarks on Exciton—Phonon Coupling and Exciton Transport

Cited by 34 publications

References 22 publications

Dynamics of Light Harvesting in Photosynthesis

Dynamics of Light Harvesting in Photosynthesis

Universal Inverse Scaling of Exciton–Exciton Annihilation Coefficient with Exciton Lifetime

Resonance energy flow dynamics of coherently delocalized excitons in biological and macromolecular systems: Recent theoretical advances and open issues

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