Abstract
Photoexcitation of the electron donor (D) within a linear, covalent donor-acceptor-acceptor molecule (D-A 1-A 2) in which A 1 = A 2 results in sub-nanosecond formation of a spin-coherent singlet radical ion pair state, 1(D +•- A 1 -•-A 2), for which the spin-spin exchange interaction is large: 2J = 79 ± 1 mT. Subsequent laser excitation of A 1 -• during the lifetime of 1(D +•-A 1 -•-A 2) rapidly produces 1(D +•-A 1-A 2 -•), which abruptly decreases 2J 3600-fold. Subsequent coherent spin evolution mixes 1(D +•-A 1-A 2 -•) with 3(D +•-A 1-A 2 -•), resulting in mixed states which display transient spin-polarized EPR transitions characteristic of a spin-correlated radical ion pair. These photodriven J-jump experiments show that it is possible to use fast laser pulses to transfer electron spin coherence between organic radical ion pairs and observe the results using an essentially background-free time-resolved EPR experiment.
| Original language | English |
|---|---|
| Pages (from-to) | 12430-12433 |
| Number of pages | 4 |
| Journal | Journal of the American Chemical Society |
| Volume | 134 |
| Issue number | 30 |
| DOIs | |
| Publication status | Published - Aug 1 2012 |
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ASJC Scopus subject areas
- Chemistry(all)
- Catalysis
- Biochemistry
- Colloid and Surface Chemistry
Cite this
Fast photodriven electron spin coherence transfer : A quantum gate based on a spin exchange J-jump. / Kobr, Lukáš; Gardner, Daniel M.; Smeigh, Amanda L.; Dyar, Scott M.; Karlen, Steven D.; Carmieli, Raanan; Wasielewski, Michael R.
In: Journal of the American Chemical Society, Vol. 134, No. 30, 01.08.2012, p. 12430-12433.Research output: Contribution to journal › Article
}
TY - JOUR
T1 - Fast photodriven electron spin coherence transfer
T2 - A quantum gate based on a spin exchange J-jump
AU - Kobr, Lukáš
AU - Gardner, Daniel M.
AU - Smeigh, Amanda L.
AU - Dyar, Scott M.
AU - Karlen, Steven D.
AU - Carmieli, Raanan
AU - Wasielewski, Michael R
PY - 2012/8/1
Y1 - 2012/8/1
N2 - Photoexcitation of the electron donor (D) within a linear, covalent donor-acceptor-acceptor molecule (D-A 1-A 2) in which A 1 = A 2 results in sub-nanosecond formation of a spin-coherent singlet radical ion pair state, 1(D +•- A 1 -•-A 2), for which the spin-spin exchange interaction is large: 2J = 79 ± 1 mT. Subsequent laser excitation of A 1 -• during the lifetime of 1(D +•-A 1 -•-A 2) rapidly produces 1(D +•-A 1-A 2 -•), which abruptly decreases 2J 3600-fold. Subsequent coherent spin evolution mixes 1(D +•-A 1-A 2 -•) with 3(D +•-A 1-A 2 -•), resulting in mixed states which display transient spin-polarized EPR transitions characteristic of a spin-correlated radical ion pair. These photodriven J-jump experiments show that it is possible to use fast laser pulses to transfer electron spin coherence between organic radical ion pairs and observe the results using an essentially background-free time-resolved EPR experiment.
AB - Photoexcitation of the electron donor (D) within a linear, covalent donor-acceptor-acceptor molecule (D-A 1-A 2) in which A 1 = A 2 results in sub-nanosecond formation of a spin-coherent singlet radical ion pair state, 1(D +•- A 1 -•-A 2), for which the spin-spin exchange interaction is large: 2J = 79 ± 1 mT. Subsequent laser excitation of A 1 -• during the lifetime of 1(D +•-A 1 -•-A 2) rapidly produces 1(D +•-A 1-A 2 -•), which abruptly decreases 2J 3600-fold. Subsequent coherent spin evolution mixes 1(D +•-A 1-A 2 -•) with 3(D +•-A 1-A 2 -•), resulting in mixed states which display transient spin-polarized EPR transitions characteristic of a spin-correlated radical ion pair. These photodriven J-jump experiments show that it is possible to use fast laser pulses to transfer electron spin coherence between organic radical ion pairs and observe the results using an essentially background-free time-resolved EPR experiment.
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U2 - 10.1021/ja305650x
DO - 10.1021/ja305650x
M3 - Article
VL - 134
SP - 12430
EP - 12433
JO - Journal of the American Chemical Society
JF - Journal of the American Chemical Society
SN - 0002-7863
IS - 30
ER -