Interaction of Photogenerated Spin Qubit Pairs with a Third Electron Spin in DNA Hairpins
The designing of tunable molecular systems that can host spin qubits is a promising strategy for advancing the development of quantum information science (QIS) applications. Photogenerated radical pairs are good spin qubit pair (SQP) candidates because they can be initialized in a pure quantum state that exhibits relatively long coherence times. DNA is a well-studied molecular system that allows for control of energetics and spatial specificity through careful design and thus serves as a tunable scaffold on which to control multispin interactions. Here, we examine a series of DNA hairpins that use naphthalenediimide (NDI) as the hairpin linker. Photoexcitation of the NDI leads to subnanosecond oxidation of guanine (G) within the duplex or a stilbenediether (Sd) end-cap to give NDI•--G•+ or NDI•--Sd•+ SQPs, respectively. A 2,2,6,6-tetramethylpiperdinyl-1-oxyl (TEMPO) stable radical is covalently attached to the hairpin at varying distances from the SQP spins. While TEMPO has a minimal effect on the SQP formation and decay dynamics, EPR spectroscopy indicates that there are significant spin-spin dipolar interactions between the SQP and TEMPO. We also demonstrate the ability to implement more complex spin manipulations of the NDI•--Sd•+-TEMPO system using pulse-EPR techniques, which is important for developing DNA hairpins for QIS applications.
| Medienart: |
E-Artikel |
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| Erscheinungsjahr: |
2021 |
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| Erschienen: |
2021 |
| Enthalten in: |
Zur Gesamtaufnahme - volume:143 |
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| Enthalten in: |
Journal of the American Chemical Society - 143(2021), 12 vom: 31. März, Seite 4625-4632 |
| Sprache: |
Englisch |
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| Beteiligte Personen: |
Lorenzo, Emmaline R [VerfasserIn] |
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| Links: |
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| Themen: |
22291-04-9 |
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| Anmerkungen: |
Date Completed 31.08.2021 Date Revised 31.08.2021 published: Print-Electronic Citation Status MEDLINE |
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| doi: |
10.1021/jacs.0c12645 |
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| funding: |
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| Förderinstitution / Projekttitel: |
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NLM322920728 |
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| 245 | 1 | 0 | |a Interaction of Photogenerated Spin Qubit Pairs with a Third Electron Spin in DNA Hairpins |
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| 500 | |a Citation Status MEDLINE | ||
| 520 | |a The designing of tunable molecular systems that can host spin qubits is a promising strategy for advancing the development of quantum information science (QIS) applications. Photogenerated radical pairs are good spin qubit pair (SQP) candidates because they can be initialized in a pure quantum state that exhibits relatively long coherence times. DNA is a well-studied molecular system that allows for control of energetics and spatial specificity through careful design and thus serves as a tunable scaffold on which to control multispin interactions. Here, we examine a series of DNA hairpins that use naphthalenediimide (NDI) as the hairpin linker. Photoexcitation of the NDI leads to subnanosecond oxidation of guanine (G) within the duplex or a stilbenediether (Sd) end-cap to give NDI•--G•+ or NDI•--Sd•+ SQPs, respectively. A 2,2,6,6-tetramethylpiperdinyl-1-oxyl (TEMPO) stable radical is covalently attached to the hairpin at varying distances from the SQP spins. While TEMPO has a minimal effect on the SQP formation and decay dynamics, EPR spectroscopy indicates that there are significant spin-spin dipolar interactions between the SQP and TEMPO. We also demonstrate the ability to implement more complex spin manipulations of the NDI•--Sd•+-TEMPO system using pulse-EPR techniques, which is important for developing DNA hairpins for QIS applications | ||
| 650 | 4 | |a Journal Article | |
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| 700 | 1 | |a Olshansky, Jacob H |e verfasserin |4 aut | |
| 700 | 1 | |a Abia, Daniel S D |e verfasserin |4 aut | |
| 700 | 1 | |a Krzyaniak, Matthew D |e verfasserin |4 aut | |
| 700 | 1 | |a Young, Ryan M |e verfasserin |4 aut | |
| 700 | 1 | |a Wasielewski, Michael R |e verfasserin |4 aut | |
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