Fast Photodriven Electron Spin Coherence Transfer: A Quantum Gate Based on a Spin Exchange J‑Jump

Photoexcitation of the electron donor (D) within a linear, covalent donor–acceptor–acceptor molecule (D-A1-A2) in which A1 = A2 results in sub-nanosecond formation of a spin-coherent singlet radical ion pair state, 1(D+•-A1 –•-A2), for which the spin–spin exchange interaction is large: 2J = 79 ± 1 m...

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Bibliographic Details
Published in:Journal of the American Chemical Society 2012-08, Vol.134 (30), p.12430-12433
Main Authors: Kobr, Lukáš, Gardner, Daniel M, Smeigh, Amanda L, Dyar, Scott M, Karlen, Steven D, Carmieli, Raanan, Wasielewski, Michael R
Format: Article
Language:English
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Summary:Photoexcitation of the electron donor (D) within a linear, covalent donor–acceptor–acceptor molecule (D-A1-A2) in which A1 = A2 results in sub-nanosecond formation of a spin-coherent singlet radical ion pair state, 1(D+•-A1 –•-A2), for which the spin–spin exchange interaction is large: 2J = 79 ± 1 mT. Subsequent laser excitation of A1 –• during the lifetime of 1(D+•-A1 –•-A2) rapidly produces 1(D+•-A1-A2 –•), which abruptly decreases 2J 3600-fold. Subsequent coherent spin evolution mixes 1(D+•-A1-A2 –•) with 3(D+•-A1-A2 –•), 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.
ISSN:0002-7863
1520-5126
DOI:10.1021/ja305650x