Coherence in Energy Transfer and Photosynthesis

Chenu, Aurélia; Scholes, Gregory D.

doi:10.1146/annurev-physchem-040214-121713

Cited by 374 publications

(415 citation statements)

References 155 publications

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“…4c, d. The complexity of theory needed to predict energy transfer depends on a balance of frequency scales, as discussed in section 'Defining and detecting coherence' , necessitating development of sophisticated theories to describe details of the energy-transfer mechanism [68][69][70][71][72] . What evidence is there that these complicated theories are necessary?…”

Section: Review Researchmentioning

confidence: 99%

Using coherence to enhance function in chemical and biophysical systems

Scholes

Fleming

Chen

et al. 2017

Nature

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572

550

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Section: Review Researchmentioning

confidence: 99%

Using coherence to enhance function in chemical and biophysical systems

Scholes

Fleming

Chen

et al. 2017

Nature

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572

550

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“…40 A highly debated point in the literature is the role of quantum mechanical coherence in the evolution of excited states in LHCs. [41][42][43] Any fluctuation of the excitonic couplings due to short range interactions coupled to thermal motion is expected to decrease the coherence and affect the exciton dynamics. 39,44,45 The aim of this paper is to evaluate the excitonic coupling between pairs of chromophores in three different LHCs and in two organic semiconductors (one amorphous and one crystalline), to achieve a broader understanding of the importance of short range interactions valid for most of the problems under current consideration.…”

Section:   a B A Bmentioning

confidence: 99%

Importance and Nature of Short-Range Excitonic Interactions in Light Harvesting Complexes and Organic Semiconductors

Fornari

Rowe

Padula

et al. 2017

J. Chem. Theory Comput.

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Copies of full items can be used for personal research or study, educational, or not-for profit purposes without prior permission or charge. Provided that the authors, title and full bibliographic details are credited, a hyperlink and/or URL is given for the original metadata page and the content is not changed in any way. Publisher's statement:"This document is the Accepted Manuscript version of a Published Work that appeared in final form in Journal of Chemical Theory and Computation. copyright © American Chemical Society after peer review and technical editing by the publisher. To access the final edited and published work http://pubs.acs.org/page/policy/articlesonrequest/index.html ." A note on versions:The version presented here may differ from the published version or, version of record, if you wish to cite this item you are advised to consult the publisher's version. Please see the 'permanent WRAP URL above for details on accessing the published version and note that access may require a subscription. AbstractThe singlet excitonic coupling between many pairs of chromophores is evaluated in three different Light Harvesting Complexes (LHCs) and two organic semiconductors (amorphous and crystalline). This large database of structures is used to assess the relative importance of short-range (exchange, overlap, orbital) and long-range (Coulombic) excitonic coupling. We find that Mulliken atomic transition charges can introduce systematic errors in the Coulombic coupling and that the dipole-dipole interaction fails to capture the true Coulombic coupling even at intermolecular distances of up to 50 Å. The non-Coulombic short range contribution to the excitonic coupling is found to represent up to ~70% of the total value for molecules in close contact, while, as expected, it is found to be negligible for dimers not in close contact. For the face-to-face dimers considered here, the sign of the short range interaction is found to correlate with the sign of the Coulombic coupling, i.e. reinforcing it when it is already strong. We conclude that for molecules in van der Waals contact the inclusion of short range effects is essential for a quantitative description of the exciton dynamics.

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“…16,18 A few examples in related self-assembled systems (porphyrins) have shown that exciton diffusion can efficiently occur by means of a coherent mechanism. 19 Recently, an octa(butyl)-substituted metal-free phthalocyanine, H2-OBPc (1,4,8,11,15,18,22,25-octabutoxy-29H,31H-phthalocyanine, see Figure 1a) has been synthesized and exhibited good crystallinity properties (1D π-stacked arrangements, see Figure 1b) in thin films. 20,21 The high degree of crystallinity of the solution-processed thin films allowed Rawat et al to investigate the correlation between long-range order and the nature of the lowest exciton states of the aggregate.…”

Section: Introductionmentioning

confidence: 99%

Exciton Dynamics in Phthalocyanine Molecular Crystals

2016

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In this paper, the exciton transport properties of an octa(butyl)-substituted metal-free phthalocyanine (H2-OBPc) molecular crystal have been explored by means of a combined computational (molecular dynamics and electronic structure calculations) and theoretical (model Hamiltonian) approximation. The excitonic couplings in phthalocyanines, where multiple quasi-degenerate excited states are present in the isolated chromophore, are computed with a multistate diabatization scheme which is able to capture both short-and long-range excitonic coupling effects. Thermal motions in phthalocyanine molecular crystals at room temperature cause substantial fluctuation of the excitonic couplings between neighboring molecules (dynamic disorder). The average values of the excitonic couplings are found to be not much smaller than the reorganization energy for the excitation energy transfer and the commonly assumed incoherent regime for this class of materials cannot be invoked. A simple but realistic model Hamiltonian is proposed to study the exciton dynamics in phthalocyanine molecular crystals or aggregates beyond the incoherent regime.2

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Coherence in Energy Transfer and Photosynthesis

Cited by 374 publications

References 155 publications

Using coherence to enhance function in chemical and biophysical systems

Using coherence to enhance function in chemical and biophysical systems

Importance and Nature of Short-Range Excitonic Interactions in Light Harvesting Complexes and Organic Semiconductors

Exciton Dynamics in Phthalocyanine Molecular Crystals

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