TY - JOUR
T1 - Zero Quantum Coherence in a Series of Covalent Spin-Correlated Radical Pairs
AU - Nelson, Jordan N.
AU - Krzyaniak, Matthew D.
AU - Horwitz, Noah E.
AU - Rugg, Brandon K.
AU - Phelan, Brian T.
AU - Wasielewski, Michael R.
N1 - Funding Information:
This work was supported by the National Science Foundation under Grant No. CHE-1565925. We thank Dr. Daniel M. Gardner for earlier synthetic efforts.
Publisher Copyright:
© 2017 American Chemical Society.
PY - 2017/3/23
Y1 - 2017/3/23
N2 - Photoinitiated subnanosecond electron transfer within covalently linked electron donor-acceptor molecules can result in the formation of a spin-correlated radical pair (SCRP) with a well-defined initial singlet spin configuration. Subsequent coherent mixing between the SCRP singlet and triplet ms = 0 spin states, the so-called zero quantum coherence (ZQC), is of potential interest in quantum information processing applications because the ZQC can be probed using pulse electron paramagnetic resonance (pulse-EPR) techniques. Here, pulse-EPR spectroscopy is utilized to examine the ZQC oscillation frequencies and ZQC dephasing in three structurally well-defined D-A systems. While transitions between the singlet and triplet ms = 0 spin states are formally forbidden (Δms = 0), they can be addressed using specific microwave pulse turning angles to map information from the ZQC onto observable single quantum coherences. In addition, by using structural variations to tune the singlet-triplet energy gap, the ZQC frequencies determined for this series of molecules indicate a stronger dependence on the electronic g-factor than on electron-nuclear hyperfine interactions.
AB - Photoinitiated subnanosecond electron transfer within covalently linked electron donor-acceptor molecules can result in the formation of a spin-correlated radical pair (SCRP) with a well-defined initial singlet spin configuration. Subsequent coherent mixing between the SCRP singlet and triplet ms = 0 spin states, the so-called zero quantum coherence (ZQC), is of potential interest in quantum information processing applications because the ZQC can be probed using pulse electron paramagnetic resonance (pulse-EPR) techniques. Here, pulse-EPR spectroscopy is utilized to examine the ZQC oscillation frequencies and ZQC dephasing in three structurally well-defined D-A systems. While transitions between the singlet and triplet ms = 0 spin states are formally forbidden (Δms = 0), they can be addressed using specific microwave pulse turning angles to map information from the ZQC onto observable single quantum coherences. In addition, by using structural variations to tune the singlet-triplet energy gap, the ZQC frequencies determined for this series of molecules indicate a stronger dependence on the electronic g-factor than on electron-nuclear hyperfine interactions.
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U2 - 10.1021/acs.jpca.7b00587
DO - 10.1021/acs.jpca.7b00587
M3 - Article
C2 - 28257610
AN - SCOPUS:85019691036
VL - 121
SP - 2241
EP - 2252
JO - Journal of Physical Chemistry A
JF - Journal of Physical Chemistry A
SN - 1089-5639
IS - 11
ER -