Fast photodriven electron spin coherence transfer: A quantum gate based on a spin exchange J-jump

Lukáš Kobr; Daniel M. Gardner; Amanda Smeigh; Scott M. Dyar; Steven D. Karlen; Raanan Carmieli; Michael R. Wasielewski

doi:10.1021/ja305650x

Fast photodriven electron spin coherence transfer: A quantum gate based on a spin exchange J-jump

Lukáš Kobr, Daniel M. Gardner, Amanda Smeigh, Scott M. Dyar, Steven D. Karlen, Raanan Carmieli, Michael R. Wasielewski

Northwestern University

Research output: Contribution to journal › Article › peer-review

25 Citations (Scopus)

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	https://doi.org/10.1021/ja305650x
Publication status	Published - Aug 1 2012

ASJC Scopus subject areas

Catalysis
Chemistry(all)
Biochemistry
Colloid and Surface Chemistry

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10.1021/ja305650x

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Fast photodriven electron spin coherence transfer : A quantum gate based on a spin exchange J-jump. / Kobr, Lukáš; Gardner, Daniel M.; Smeigh, Amanda; 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 › peer-review

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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.",

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