Powered by OpenAIRE graph
Found an issue? Give us feedback
image/svg+xml art designer at PLoS, modified by Wikipedia users Nina, Beao, JakobVoss, and AnonMoos Open Access logo, converted into svg, designed by PLoS. This version with transparent background. http://commons.wikimedia.org/wiki/File:Open_Access_logo_PLoS_white.svg art designer at PLoS, modified by Wikipedia users Nina, Beao, JakobVoss, and AnonMoos http://www.plos.org/ The Journal of Physi...arrow_drop_down
image/svg+xml art designer at PLoS, modified by Wikipedia users Nina, Beao, JakobVoss, and AnonMoos Open Access logo, converted into svg, designed by PLoS. This version with transparent background. http://commons.wikimedia.org/wiki/File:Open_Access_logo_PLoS_white.svg art designer at PLoS, modified by Wikipedia users Nina, Beao, JakobVoss, and AnonMoos http://www.plos.org/
The Journal of Physical Chemistry A
Article . 2023 . Peer-reviewed
License: CC BY
Data sources: Crossref
image/svg+xml art designer at PLoS, modified by Wikipedia users Nina, Beao, JakobVoss, and AnonMoos Open Access logo, converted into svg, designed by PLoS. This version with transparent background. http://commons.wikimedia.org/wiki/File:Open_Access_logo_PLoS_white.svg art designer at PLoS, modified by Wikipedia users Nina, Beao, JakobVoss, and AnonMoos http://www.plos.org/
image/svg+xml art designer at PLoS, modified by Wikipedia users Nina, Beao, JakobVoss, and AnonMoos Open Access logo, converted into svg, designed by PLoS. This version with transparent background. http://commons.wikimedia.org/wiki/File:Open_Access_logo_PLoS_white.svg art designer at PLoS, modified by Wikipedia users Nina, Beao, JakobVoss, and AnonMoos http://www.plos.org/
image/svg+xml art designer at PLoS, modified by Wikipedia users Nina, Beao, JakobVoss, and AnonMoos Open Access logo, converted into svg, designed by PLoS. This version with transparent background. http://commons.wikimedia.org/wiki/File:Open_Access_logo_PLoS_white.svg art designer at PLoS, modified by Wikipedia users Nina, Beao, JakobVoss, and AnonMoos http://www.plos.org/
https://dx.doi.org/10.48550/ar...
Article . 2022
License: CC BY
Data sources: Datacite
versions View all 7 versions
addClaim

Photoexcited State Dynamics and Singlet Fission in Carotenoids

Authors: Dilhan Manawadu; Timothy N. Georges; William Barford;

Photoexcited State Dynamics and Singlet Fission in Carotenoids

Abstract

We describe our dynamical simulations of the excited states of the carotenoid, neurosporene, following its photoexcitation into the 'bright' (nominally $1^1B_u^+$) state. We employ the adaptive tDMRG method on the UV model of $π$-conjugated electrons and use the Ehrenfest equations of motion to simulate the coupled nuclei dynamics. To account for the experimental and theoretical uncertainty in the relative energetic ordering of the nominal $1^1B_u^+$ and $2^1A_g^-$ states at the Franck-Condon point, we consider two parameter sets. In both cases there is ultrafast internal conversion from the 'bright' state to a 'dark' singlet triplet-pair state. We make a direct connection from our predictions to experimental observables by calculating the transient absorption. For the case of direct $1^1B_u^+$ to $2^1A_g^-$ internal conversion, we show that the dominant transition at ca. 2 eV, being close to but lower in energy than the $T_1$ to $T_1^*$ transition, can be attributed to the $2^1A_g^-$ component of $S_1$. Moreover, we show that it is the charge-transfer exciton component of the $2^1A_g^-$ state that is responsible for this transition, and not its triplet-pair component. We next discuss the microscopic mechanism of 'bright' to 'dark' state internal conversion, emphasising that this occurs via the exciton components of both states. Finally, we describe a mechanism whereby the strongly bound intrachain triplet-pairs of the 'dark' state may undergo interchain exothermic dissociation. We predict that this is only possible if the molecules are twisted in their ground states. The computational methodology underlying the calculations described here is explained in our companion paper, $\textit{Dynamical simulations of carotenoid photoexcited states using density matrix renormalization group techniques}$, D. Manawadu, D. J. Valentine, and W. Barford, $\textit{J. Chem. Theo. Comp.}$ (2023).

31 pages, 11 figures

Country
United Kingdom
Related Organizations
Keywords

Chemical Physics (physics.chem-ph), Physics - Chemical Physics, FOS: Physical sciences

  • BIP!
    Impact byBIP!
    selected citations
    These citations are derived from selected sources.
    This is an alternative to the "Influence" indicator, which also reflects the overall/total impact of an article in the research community at large, based on the underlying citation network (diachronically).
    12
    popularity
    This indicator reflects the "current" impact/attention (the "hype") of an article in the research community at large, based on the underlying citation network.
    Top 10%
    influence
    This indicator reflects the overall/total impact of an article in the research community at large, based on the underlying citation network (diachronically).
    Average
    impulse
    This indicator reflects the initial momentum of an article directly after its publication, based on the underlying citation network.
    Top 10%
Powered by OpenAIRE graph
Found an issue? Give us feedback
selected citations
These citations are derived from selected sources.
This is an alternative to the "Influence" indicator, which also reflects the overall/total impact of an article in the research community at large, based on the underlying citation network (diachronically).
BIP!Citations provided by BIP!
popularity
This indicator reflects the "current" impact/attention (the "hype") of an article in the research community at large, based on the underlying citation network.
BIP!Popularity provided by BIP!
influence
This indicator reflects the overall/total impact of an article in the research community at large, based on the underlying citation network (diachronically).
BIP!Influence provided by BIP!
impulse
This indicator reflects the initial momentum of an article directly after its publication, based on the underlying citation network.
BIP!Impulse provided by BIP!
12
Top 10%
Average
Top 10%
Green
hybrid