Resolving Energy and Electron Transfer Processes in Dyads With the Help of Global and Target AnalysisaaThis chapter extends the data analysis and modelling of Pillai et al. (2013)

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

Research output: Contribution to journalArticle

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 S1 and S1 states.

Original languageEnglish
JournalAdvances in Botanical Research
DOIs
Publication statusAccepted/In press - 2016

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energy transfer
fullerene
electron transfer
data analysis
carotenoids
porphyrins
deterioration
case studies
energy
methodology

Keywords

  • Electron transfer
  • Excited state absorption
  • Excited state energy transfer
  • Global analysis
  • Kinetic modelling
  • Target analysis
  • Transient absorption spectroscopy

ASJC Scopus subject areas

  • Plant Science

Cite this

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title = "Resolving Energy and Electron Transfer Processes in Dyads With the Help of Global and Target AnalysisaaThis chapter extends the data analysis and modelling of Pillai et al. (2013)",
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 S1 and S1 states.",
keywords = "Electron transfer, Excited state absorption, Excited state energy transfer, Global analysis, Kinetic modelling, Target analysis, Transient absorption spectroscopy",
author = "{van Stokkum}, {I. H M} and J. Ravensbergen and Snellenburg, {J. J.} and {van Grondelle}, R. and S. Pillai and Moore, {Thomas A} and Gust, {John Devens} and Moore, {Ana L} and Kennis, {J. T M}",
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T1 - Resolving Energy and Electron Transfer Processes in Dyads With the Help of Global and Target AnalysisaaThis chapter extends the data analysis and modelling of Pillai et al. (2013)

AU - van Stokkum, I. H M

AU - Ravensbergen, J.

AU - Snellenburg, J. J.

AU - van Grondelle, R.

AU - Pillai, S.

AU - Moore, Thomas A

AU - Gust, John Devens

AU - Moore, Ana L

AU - Kennis, J. T M

PY - 2016

Y1 - 2016

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 S1 and S1 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 S1 and S1 states.

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