Resolving Energy and Electron Transfer Processes in Dyads With the Help of Global and Target Analysis

I.H.M. van Stokkum, J. Ravensbergen, J.J. Snellenburg, R. van Grondelle, S. Pillai, T.A. Moore, D. Gust, A.L. Moore, J.T.M. Kennis

Research output: Chapter in Book / Report / Conference proceedingChapterAcademicpeer-review

Abstract

In any photosynthetic/photocatalytic device, multiple steps are required between the arrival of a solar photon and the formation of a stable product. Here we explain and demonstrate the target analysis methodology to develop minimal models, identify the steps and estimate the parameters that characterize energy converting devices. With this modelling tool the molecular mechanisms of the loss processes can be identified and quantified. This can then inspire photosynthetic device optimization by precisely targeting those sites involved in the most significant losses. Two case studies of recently published measurements (Pillai et al., 2013) on a carotenoporphyrin dyad and a carotenofullerene dyad are modelled in depth. After carotenoid excitation, no excited state energy transfer (EET) to porphyrin was found, but EET from carotenoid hot S1 to the fullerene moiety occurred with a rate of 1.6/ps. The total radical pair yields of these dyads were found to be, respectively, 46% and 79%. Out of these 79%, 31% were due to electron transfer from the fullerene excited state. The triplet yields were 3.8% and 4.6%. The remainder of the excitations decay to the ground state from the carotenoid hot S-1 and S-1 states.
Original languageEnglish
Title of host publicationArtificial Photosynthesis
EditorsR. Bruno
Place of PublicationAmsterdam
PublisherAdvances in Botanical Researc
Pages169-192
Volume79
ISBN (Print)978-0-12-803325-8; 978-0-12-80
DOIs
Publication statusPublished - 2016

Publication series

Name79

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Carotenoids
Fullerenes
Excited states
Energy transfer
Electrons
Porphyrins
Ground state
Photons

Cite this

van Stokkum, I. H. M., Ravensbergen, J., Snellenburg, J. J., van Grondelle, R., Pillai, S., Moore, T. A., ... Kennis, J. T. M. (2016). Resolving Energy and Electron Transfer Processes in Dyads With the Help of Global and Target Analysis. In R. Bruno (Ed.), Artificial Photosynthesis (Vol. 79, pp. 169-192). (79). Amsterdam: Advances in Botanical Researc. https://doi.org/10.1016/bs.abr.2016.04.003
van Stokkum, I.H.M. ; Ravensbergen, J. ; Snellenburg, J.J. ; van Grondelle, R. ; Pillai, S. ; Moore, T.A. ; Gust, D. ; Moore, A.L. ; Kennis, J.T.M. / Resolving Energy and Electron Transfer Processes in Dyads With the Help of Global and Target Analysis. Artificial Photosynthesis. editor / R. Bruno. Vol. 79 Amsterdam : Advances in Botanical Researc, 2016. pp. 169-192 (79).
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abstract = "In any photosynthetic/photocatalytic device, multiple steps are required between the arrival of a solar photon and the formation of a stable product. Here we explain and demonstrate the target analysis methodology to develop minimal models, identify the steps and estimate the parameters that characterize energy converting devices. With this modelling tool the molecular mechanisms of the loss processes can be identified and quantified. This can then inspire photosynthetic device optimization by precisely targeting those sites involved in the most significant losses. Two case studies of recently published measurements (Pillai et al., 2013) on a carotenoporphyrin dyad and a carotenofullerene dyad are modelled in depth. After carotenoid excitation, no excited state energy transfer (EET) to porphyrin was found, but EET from carotenoid hot S1 to the fullerene moiety occurred with a rate of 1.6/ps. The total radical pair yields of these dyads were found to be, respectively, 46{\%} and 79{\%}. Out of these 79{\%}, 31{\%} were due to electron transfer from the fullerene excited state. The triplet yields were 3.8{\%} and 4.6{\%}. The remainder of the excitations decay to the ground state from the carotenoid hot S-1 and S-1 states.",
author = "{van Stokkum}, I.H.M. and J. Ravensbergen and J.J. Snellenburg and {van Grondelle}, R. and S. Pillai and T.A. Moore and D. Gust and A.L. Moore and J.T.M. Kennis",
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van Stokkum, IHM, Ravensbergen, J, Snellenburg, JJ, van Grondelle, R, Pillai, S, Moore, TA, Gust, D, Moore, AL & Kennis, JTM 2016, Resolving Energy and Electron Transfer Processes in Dyads With the Help of Global and Target Analysis. in R Bruno (ed.), Artificial Photosynthesis. vol. 79, 79, Advances in Botanical Researc, Amsterdam, pp. 169-192. https://doi.org/10.1016/bs.abr.2016.04.003

Resolving Energy and Electron Transfer Processes in Dyads With the Help of Global and Target Analysis. / van Stokkum, I.H.M.; Ravensbergen, J.; Snellenburg, J.J.; van Grondelle, R.; Pillai, S.; Moore, T.A.; Gust, D.; Moore, A.L.; Kennis, J.T.M.

Artificial Photosynthesis. ed. / R. Bruno. Vol. 79 Amsterdam : Advances in Botanical Researc, 2016. p. 169-192 (79).

Research output: Chapter in Book / Report / Conference proceedingChapterAcademicpeer-review

TY - CHAP

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AU - van Stokkum, I.H.M.

AU - Ravensbergen, J.

AU - Snellenburg, J.J.

AU - van Grondelle, R.

AU - Pillai, S.

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AU - Kennis, J.T.M.

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N2 - In any photosynthetic/photocatalytic device, multiple steps are required between the arrival of a solar photon and the formation of a stable product. Here we explain and demonstrate the target analysis methodology to develop minimal models, identify the steps and estimate the parameters that characterize energy converting devices. With this modelling tool the molecular mechanisms of the loss processes can be identified and quantified. This can then inspire photosynthetic device optimization by precisely targeting those sites involved in the most significant losses. Two case studies of recently published measurements (Pillai et al., 2013) on a carotenoporphyrin dyad and a carotenofullerene dyad are modelled in depth. After carotenoid excitation, no excited state energy transfer (EET) to porphyrin was found, but EET from carotenoid hot S1 to the fullerene moiety occurred with a rate of 1.6/ps. The total radical pair yields of these dyads were found to be, respectively, 46% and 79%. Out of these 79%, 31% were due to electron transfer from the fullerene excited state. The triplet yields were 3.8% and 4.6%. The remainder of the excitations decay to the ground state from the carotenoid hot S-1 and S-1 states.

AB - In any photosynthetic/photocatalytic device, multiple steps are required between the arrival of a solar photon and the formation of a stable product. Here we explain and demonstrate the target analysis methodology to develop minimal models, identify the steps and estimate the parameters that characterize energy converting devices. With this modelling tool the molecular mechanisms of the loss processes can be identified and quantified. This can then inspire photosynthetic device optimization by precisely targeting those sites involved in the most significant losses. Two case studies of recently published measurements (Pillai et al., 2013) on a carotenoporphyrin dyad and a carotenofullerene dyad are modelled in depth. After carotenoid excitation, no excited state energy transfer (EET) to porphyrin was found, but EET from carotenoid hot S1 to the fullerene moiety occurred with a rate of 1.6/ps. The total radical pair yields of these dyads were found to be, respectively, 46% and 79%. Out of these 79%, 31% were due to electron transfer from the fullerene excited state. The triplet yields were 3.8% and 4.6%. The remainder of the excitations decay to the ground state from the carotenoid hot S-1 and S-1 states.

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M3 - Chapter

SN - 978-0-12-803325-8; 978-0-12-80

VL - 79

T3 - 79

SP - 169

EP - 192

BT - Artificial Photosynthesis

A2 - Bruno, R.

PB - Advances in Botanical Researc

CY - Amsterdam

ER -

van Stokkum IHM, Ravensbergen J, Snellenburg JJ, van Grondelle R, Pillai S, Moore TA et al. Resolving Energy and Electron Transfer Processes in Dyads With the Help of Global and Target Analysis. In Bruno R, editor, Artificial Photosynthesis. Vol. 79. Amsterdam: Advances in Botanical Researc. 2016. p. 169-192. (79). https://doi.org/10.1016/bs.abr.2016.04.003