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Detecting chirality-induced spin selectivity in chromophore-linked DNA hairpins using photogenerated radical pairs.

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Title: Detecting chirality-induced spin selectivity in chromophore-linked DNA hairpins using photogenerated radical pairs.
Authors: Latawiec, Elisabeth I.1, Chiesa, Alessandro2,3,4, Yunfan Qiu1, Tcyrulnikov, Nikolai A.1, Young, Ryan M.1, Carretta, Stefano2,3,4 stefano.carretta@unipr.it, Krzyaniak, Matthew D.1 mdkrzyaniak@northwestern.edu, Wasielewski, Michael R.1 m-wasielewski@northwestern.edu
Source: Proceedings of the National Academy of Sciences of the United States of America. 8/12/2025, Vol. 122 Issue 32, p1-7. 31p.
Subjects: Magnetic flux density, Electron paramagnetic resonance, Base pairs, Polarized electrons, Electron spin
Abstract: Chirality-induced spin selectivity (CISS) results in spin polarization of electrons transmitted through chiral molecules and materials. Since CISS results in spin polarization even at room temperature, it affords the possibility of using it to develop quantum technologies that can operate under ambient conditions. We have shown previously that photo-driven hole transfer within DNA hairpins provides a facile route to generate spin-correlated radical pairs (SCRPs). To study the effect of CISS on the spin dynamics of SCRPs in DNA hairpins, we prepared a series of electron donor-chiral bridge-acceptor molecules where the chiral bridge is a B-form DNA helix consisting of 4 to 6 base pairs. Naphthalene-1,8:4,5-bis(dicarboximide) (NDI) serves as the hairpin linker chromophore and electron acceptor. Photoexcitation of NDI results in rapid hole transfer through the π-stacked purine bases of the DNA and trapping of the hole on a terminal stilbene diether (Sd) to generate the NDI•-- Sd•+ SCRP. Time-resolved electron paramagnetic resonance spectra of the SCRPs at X- (9.6 GHz), Q- (34 GHz), and W- (94 GHz) bands show that the CISS effect imparts significant triplet character to the SCRP. We do not observe a significant dependence of CISS on DNA length, likely resulting from hole delocalization over the guanine bases in the G-tract. Interestingly, we find that the CISS contribution significantly increases with magnetic field strength. These findings should be considered in any future modeling of CISS. [ABSTRACT FROM AUTHOR]
Copyright of Proceedings of the National Academy of Sciences of the United States of America is the property of National Academy of Sciences and its content may not be copied or emailed to multiple sites without the copyright holder's express written permission. Additionally, content may not be used with any artificial intelligence tools or machine learning technologies. However, users may print, download, or email articles for individual use. This abstract may be abridged. No warranty is given about the accuracy of the copy. Users should refer to the original published version of the material for the full abstract. (Copyright applies to all Abstracts.)
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  Label: Title
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  Data: Detecting chirality-induced spin selectivity in chromophore-linked DNA hairpins using photogenerated radical pairs.
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  Data: <searchLink fieldCode="AR" term="%22Latawiec%2C+Elisabeth+I%2E%22">Latawiec, Elisabeth I.</searchLink><relatesTo>1</relatesTo><br /><searchLink fieldCode="AR" term="%22Chiesa%2C+Alessandro%22">Chiesa, Alessandro</searchLink><relatesTo>2,3,4</relatesTo><br /><searchLink fieldCode="AR" term="%22Yunfan+Qiu%22">Yunfan Qiu</searchLink><relatesTo>1</relatesTo><br /><searchLink fieldCode="AR" term="%22Tcyrulnikov%2C+Nikolai+A%2E%22">Tcyrulnikov, Nikolai A.</searchLink><relatesTo>1</relatesTo><br /><searchLink fieldCode="AR" term="%22Young%2C+Ryan+M%2E%22">Young, Ryan M.</searchLink><relatesTo>1</relatesTo><br /><searchLink fieldCode="AR" term="%22Carretta%2C+Stefano%22">Carretta, Stefano</searchLink><relatesTo>2,3,4</relatesTo><i> stefano.carretta@unipr.it</i><br /><searchLink fieldCode="AR" term="%22Krzyaniak%2C+Matthew+D%2E%22">Krzyaniak, Matthew D.</searchLink><relatesTo>1</relatesTo><i> mdkrzyaniak@northwestern.edu</i><br /><searchLink fieldCode="AR" term="%22Wasielewski%2C+Michael+R%2E%22">Wasielewski, Michael R.</searchLink><relatesTo>1</relatesTo><i> m-wasielewski@northwestern.edu</i>
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  Data: <searchLink fieldCode="JN" term="%22Proceedings+of+the+National+Academy+of+Sciences+of+the+United+States+of+America%22">Proceedings of the National Academy of Sciences of the United States of America</searchLink>. 8/12/2025, Vol. 122 Issue 32, p1-7. 31p.
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  Data: <searchLink fieldCode="DE" term="%22Magnetic+flux+density%22">Magnetic flux density</searchLink><br /><searchLink fieldCode="DE" term="%22Electron+paramagnetic+resonance%22">Electron paramagnetic resonance</searchLink><br /><searchLink fieldCode="DE" term="%22Base+pairs%22">Base pairs</searchLink><br /><searchLink fieldCode="DE" term="%22Polarized+electrons%22">Polarized electrons</searchLink><br /><searchLink fieldCode="DE" term="%22Electron+spin%22">Electron spin</searchLink>
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  Label: Abstract
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  Data: Chirality-induced spin selectivity (CISS) results in spin polarization of electrons transmitted through chiral molecules and materials. Since CISS results in spin polarization even at room temperature, it affords the possibility of using it to develop quantum technologies that can operate under ambient conditions. We have shown previously that photo-driven hole transfer within DNA hairpins provides a facile route to generate spin-correlated radical pairs (SCRPs). To study the effect of CISS on the spin dynamics of SCRPs in DNA hairpins, we prepared a series of electron donor-chiral bridge-acceptor molecules where the chiral bridge is a B-form DNA helix consisting of 4 to 6 base pairs. Naphthalene-1,8:4,5-bis(dicarboximide) (NDI) serves as the hairpin linker chromophore and electron acceptor. Photoexcitation of NDI results in rapid hole transfer through the π-stacked purine bases of the DNA and trapping of the hole on a terminal stilbene diether (Sd) to generate the NDI•-- Sd•+ SCRP. Time-resolved electron paramagnetic resonance spectra of the SCRPs at X- (9.6 GHz), Q- (34 GHz), and W- (94 GHz) bands show that the CISS effect imparts significant triplet character to the SCRP. We do not observe a significant dependence of CISS on DNA length, likely resulting from hole delocalization over the guanine bases in the G-tract. Interestingly, we find that the CISS contribution significantly increases with magnetic field strength. These findings should be considered in any future modeling of CISS. [ABSTRACT FROM AUTHOR]
– Name: AbstractSuppliedCopyright
  Label:
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  Data: <i>Copyright of Proceedings of the National Academy of Sciences of the United States of America is the property of National Academy of Sciences and its content may not be copied or emailed to multiple sites without the copyright holder's express written permission. Additionally, content may not be used with any artificial intelligence tools or machine learning technologies. However, users may print, download, or email articles for individual use. This abstract may be abridged. No warranty is given about the accuracy of the copy. Users should refer to the original published version of the material for the full abstract.</i> (Copyright applies to all Abstracts.)
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        Value: 10.1073/pnas.2515120122
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      – Code: eng
        Text: English
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        PageCount: 31
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    Subjects:
      – SubjectFull: Magnetic flux density
        Type: general
      – SubjectFull: Electron paramagnetic resonance
        Type: general
      – SubjectFull: Base pairs
        Type: general
      – SubjectFull: Polarized electrons
        Type: general
      – SubjectFull: Electron spin
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      – TitleFull: Detecting chirality-induced spin selectivity in chromophore-linked DNA hairpins using photogenerated radical pairs.
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              Text: 8/12/2025
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              Y: 2025
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