TY - JOUR

T1 - J-Resonance Line Shape of Magnetic Field-Affected Reaction Yield Spectrum from Charge Recombination in a Linked Donor-Acceptor Dyad

AU - Steiner, Ulrich E.

AU - Schäfer, Julian

AU - Lukzen, Nikita N.

AU - Lambert, Christoph

N1 - Publisher Copyright: © 2018 American Chemical Society.

PY - 2018/6/7

Y1 - 2018/6/7

N2 - Magnetic field effects (MFEs) allow detailed insight into spin conversion processes of radical pairs that are formed, for example, in all charge separation processes, and are supposed to play the key role in avian navigation. In this work, the MFE of charge recombination in the charge-separated state of a rigid donor-bridge-acceptor dyad was analyzed by a classical and a quantum theoretical model and represents a paradigm case of understanding spin chemistry with unprecedented detail. The MFE is represented by magnetic field-affected reaction yield (MARY) spectra that exhibit a sharp resonance, resulting from S/T level crossing as the Zeeman splitting equals twice the exchange interaction. Although in the classical kinetic model, the spin conversion processes between the four singlet and triplet substates are shown for the first time to obey an identical generalized energy dependence, quantum theory proves that the MARY resonance line is composed of relaxation, coherent hyperfine induced spin mixing, and S/T dephasing contributions.

AB - Magnetic field effects (MFEs) allow detailed insight into spin conversion processes of radical pairs that are formed, for example, in all charge separation processes, and are supposed to play the key role in avian navigation. In this work, the MFE of charge recombination in the charge-separated state of a rigid donor-bridge-acceptor dyad was analyzed by a classical and a quantum theoretical model and represents a paradigm case of understanding spin chemistry with unprecedented detail. The MFE is represented by magnetic field-affected reaction yield (MARY) spectra that exhibit a sharp resonance, resulting from S/T level crossing as the Zeeman splitting equals twice the exchange interaction. Although in the classical kinetic model, the spin conversion processes between the four singlet and triplet substates are shown for the first time to obey an identical generalized energy dependence, quantum theory proves that the MARY resonance line is composed of relaxation, coherent hyperfine induced spin mixing, and S/T dephasing contributions.

UR - http://www.scopus.com/inward/record.url?scp=85047059681&partnerID=8YFLogxK

U2 - 10.1021/acs.jpcc.8b02904

DO - 10.1021/acs.jpcc.8b02904

M3 - Article

AN - SCOPUS:85047059681

VL - 122

SP - 11701

EP - 11708

JO - Journal of Physical Chemistry C

JF - Journal of Physical Chemistry C

SN - 1932-7447

IS - 22

ER -