Univ. of California, Berkeley, CA (United States); Lawrence Berkeley National Laboratory (LBNL), Berkeley, CA (United States); Kavli Energy NanoScience Institute, Berkeley, CA (United States)
In this paper, we outline a physically motivated framework for describing spin-selective recombination processes in chiral systems, from which we derive spin-selective reaction operators for recombination reactions of donor–bridge–acceptor molecules, where the electron transfer is mediated by chirality and spin–orbit coupling. In general, the recombination process is selective only for spin-coherence between singlet and triplet states, and it is not, in general, selective for spin polarization. We find that spin polarization selectivity only arises in hopping-mediated electron transfer. We describe how this effective spin-polarization selectivity is a consequence of spin-polarization generated transiently in the intermediate state. Furthermore, the recombination process also augments the coherent spin dynamics of the charge separated state, which is found to have a significant effect on the recombination dynamics and to destroy any long-lived spin polarization. Although we only consider a simple donor–bridge–acceptor system, the framework we present here can be straightforwardly extended to describe spin-selective recombination processes in more complex systems.
Fay, Thomas Patrick and Limmer, David T.. "Spin selective charge recombination in chiral donor-bridge-acceptor triads." Journal of Chemical Physics, vol. 158, no. 19, May. 2023. https://doi.org/10.1063/5.0150269
Fay, Thomas Patrick, & Limmer, David T. (2023). Spin selective charge recombination in chiral donor-bridge-acceptor triads. Journal of Chemical Physics, 158(19). https://doi.org/10.1063/5.0150269
Fay, Thomas Patrick, and Limmer, David T., "Spin selective charge recombination in chiral donor-bridge-acceptor triads," Journal of Chemical Physics 158, no. 19 (2023), https://doi.org/10.1063/5.0150269
@article{osti_2305342,
author = {Fay, Thomas Patrick and Limmer, David T.},
title = {Spin selective charge recombination in chiral donor-bridge-acceptor triads},
annote = {In this paper, we outline a physically motivated framework for describing spin-selective recombination processes in chiral systems, from which we derive spin-selective reaction operators for recombination reactions of donor–bridge–acceptor molecules, where the electron transfer is mediated by chirality and spin–orbit coupling. In general, the recombination process is selective only for spin-coherence between singlet and triplet states, and it is not, in general, selective for spin polarization. We find that spin polarization selectivity only arises in hopping-mediated electron transfer. We describe how this effective spin-polarization selectivity is a consequence of spin-polarization generated transiently in the intermediate state. Furthermore, the recombination process also augments the coherent spin dynamics of the charge separated state, which is found to have a significant effect on the recombination dynamics and to destroy any long-lived spin polarization. Although we only consider a simple donor–bridge–acceptor system, the framework we present here can be straightforwardly extended to describe spin-selective recombination processes in more complex systems.},
doi = {10.1063/5.0150269},
url = {https://www.osti.gov/biblio/2305342},
journal = {Journal of Chemical Physics},
issn = {ISSN 0021-9606},
number = {19},
volume = {158},
place = {United States},
publisher = {American Institute of Physics (AIP)},
year = {2023},
month = {05}}
Philosophical Transactions of the Royal Society of London. Series A: Mathematical, Physical and Engineering Sciences, Vol. 362, Issue 1825https://doi.org/10.1098/rsta.2004.1459