Abstract
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.
| Original language | English |
|---|---|
| Pages (from-to) | 2241-2252 |
| Number of pages | 12 |
| Journal | Journal of Physical Chemistry A |
| Volume | 121 |
| Issue number | 11 |
| DOIs | |
| Publication status | Published - Mar 23 2017 |
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ASJC Scopus subject areas
- Physical and Theoretical Chemistry
Cite this
Zero Quantum Coherence in a Series of Covalent Spin-Correlated Radical Pairs. / Nelson, Jordan N.; Krzyaniak, Matthew D.; Horwitz, Noah E.; Rugg, Brandon K.; Phelan, Brian T.; Wasielewski, Michael R.
In: Journal of Physical Chemistry A, Vol. 121, No. 11, 23.03.2017, p. 2241-2252.Research output: Contribution to journal › Article
}
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
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
VL - 121
SP - 2241
EP - 2252
JO - Journal of Physical Chemistry A
JF - Journal of Physical Chemistry A
SN - 1089-5639
IS - 11
ER -