Spin-selective recombination reactions of radical pairs

Experimental test of validity of reaction operators

Kiminori Maeda, Paul Liddell, John Devens Gust, P. J. Hore

Research output: Contribution to journalArticle

9 Citations (Scopus)

Abstract

Spin-selective reactions of radical pairs are conventionally modelled using an approach that dates back to the 1970s [R. Haberkorn, Mol. Phys. 32, 1491 (1976)]. An alternative approach based on the theory of quantum measurements has recently been suggested [J. A. Jones and P. J. Hore, Chem. Phys. Lett. 488, 90 (2010)]. We present here the first experimental attempt to discriminate between the two models. Pulsed electron paramagnetic resonance spectroscopy has been used to investigate intramolecular electron transfer in the radical pair form of a carotenoid-porphyrin-fullerene molecular triad. The rate of spin-spin relaxation of the fullerene radical in the triad was found to be inconsistent with the quantum measurement description of the spin-selective kinetics, and in accord with the conventional model when combined with spin-dephasing caused by rotational modulation of the anisotropic g-tensor of the fullerene radical.

Original languageEnglish
Article number234309
JournalJournal of Chemical Physics
Volume139
Issue number23
DOIs
Publication statusPublished - Dec 21 2013

Fingerprint

Fullerenes
recombination reactions
operators
fullerenes
Porphyrins
Carotenoids
Tensors
Paramagnetic resonance
carotenoids
Modulation
Spectroscopy
Kinetics
Electrons
porphyrins
electron paramagnetic resonance
electron transfer
tensors
modulation
kinetics
spectroscopy

ASJC Scopus subject areas

  • Physics and Astronomy(all)
  • Physical and Theoretical Chemistry

Cite this

Spin-selective recombination reactions of radical pairs : Experimental test of validity of reaction operators. / Maeda, Kiminori; Liddell, Paul; Gust, John Devens; Hore, P. J.

In: Journal of Chemical Physics, Vol. 139, No. 23, 234309, 21.12.2013.

Research output: Contribution to journalArticle

@article{2b747d4487ce452b9a8cb1144955c437,
title = "Spin-selective recombination reactions of radical pairs: Experimental test of validity of reaction operators",
abstract = "Spin-selective reactions of radical pairs are conventionally modelled using an approach that dates back to the 1970s [R. Haberkorn, Mol. Phys. 32, 1491 (1976)]. An alternative approach based on the theory of quantum measurements has recently been suggested [J. A. Jones and P. J. Hore, Chem. Phys. Lett. 488, 90 (2010)]. We present here the first experimental attempt to discriminate between the two models. Pulsed electron paramagnetic resonance spectroscopy has been used to investigate intramolecular electron transfer in the radical pair form of a carotenoid-porphyrin-fullerene molecular triad. The rate of spin-spin relaxation of the fullerene radical in the triad was found to be inconsistent with the quantum measurement description of the spin-selective kinetics, and in accord with the conventional model when combined with spin-dephasing caused by rotational modulation of the anisotropic g-tensor of the fullerene radical.",
author = "Kiminori Maeda and Paul Liddell and Gust, {John Devens} and Hore, {P. J.}",
year = "2013",
month = "12",
day = "21",
doi = "10.1063/1.4844355",
language = "English",
volume = "139",
journal = "Journal of Chemical Physics",
issn = "0021-9606",
publisher = "American Institute of Physics Publising LLC",
number = "23",

}

TY - JOUR

T1 - Spin-selective recombination reactions of radical pairs

T2 - Experimental test of validity of reaction operators

AU - Maeda, Kiminori

AU - Liddell, Paul

AU - Gust, John Devens

AU - Hore, P. J.

PY - 2013/12/21

Y1 - 2013/12/21

N2 - Spin-selective reactions of radical pairs are conventionally modelled using an approach that dates back to the 1970s [R. Haberkorn, Mol. Phys. 32, 1491 (1976)]. An alternative approach based on the theory of quantum measurements has recently been suggested [J. A. Jones and P. J. Hore, Chem. Phys. Lett. 488, 90 (2010)]. We present here the first experimental attempt to discriminate between the two models. Pulsed electron paramagnetic resonance spectroscopy has been used to investigate intramolecular electron transfer in the radical pair form of a carotenoid-porphyrin-fullerene molecular triad. The rate of spin-spin relaxation of the fullerene radical in the triad was found to be inconsistent with the quantum measurement description of the spin-selective kinetics, and in accord with the conventional model when combined with spin-dephasing caused by rotational modulation of the anisotropic g-tensor of the fullerene radical.

AB - Spin-selective reactions of radical pairs are conventionally modelled using an approach that dates back to the 1970s [R. Haberkorn, Mol. Phys. 32, 1491 (1976)]. An alternative approach based on the theory of quantum measurements has recently been suggested [J. A. Jones and P. J. Hore, Chem. Phys. Lett. 488, 90 (2010)]. We present here the first experimental attempt to discriminate between the two models. Pulsed electron paramagnetic resonance spectroscopy has been used to investigate intramolecular electron transfer in the radical pair form of a carotenoid-porphyrin-fullerene molecular triad. The rate of spin-spin relaxation of the fullerene radical in the triad was found to be inconsistent with the quantum measurement description of the spin-selective kinetics, and in accord with the conventional model when combined with spin-dephasing caused by rotational modulation of the anisotropic g-tensor of the fullerene radical.

UR - http://www.scopus.com/inward/record.url?scp=84906044948&partnerID=8YFLogxK

UR - http://www.scopus.com/inward/citedby.url?scp=84906044948&partnerID=8YFLogxK

U2 - 10.1063/1.4844355

DO - 10.1063/1.4844355

M3 - Article

VL - 139

JO - Journal of Chemical Physics

JF - Journal of Chemical Physics

SN - 0021-9606

IS - 23

M1 - 234309

ER -