Journal
NANO LETTERS
Volume 20, Issue 2, Pages 1218-1225Publisher
AMER CHEMICAL SOC
DOI: 10.1021/acs.nanolett.9b04622
Keywords
Chiral-induced spin selectivity (CISS) effect; electron dichroism; molecular spintronics; photoelectron spectroscopy; DNA nanotechnology
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Funding
- National Science Foundation ECCS [1509794]
- National Institute on Drug Abuse [DA045550]
- National Science Foundation DMR [1610538]
- Direct For Mathematical & Physical Scien
- Division Of Materials Research [1610538] Funding Source: National Science Foundation
- Directorate For Engineering [1509794] Funding Source: National Science Foundation
- Div Of Electrical, Commun & Cyber Sys [1509794] Funding Source: National Science Foundation
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Spin-dependent and enantioselective electron-molecule scattering occurs in photoelectron transmission through chiral molecular films. This spin selectivity leads to electron spin filtering by molecular helices, with increasing magnitude concomitant with increasing numbers of helical turns. Using ultraviolet photoelectron spectroscopy, we measured spinselective surface charging accompanying photoemission from ferromagnetic substrates functionalized with monolayers of mercurated DNA hairpins that constitute only one helical turn. Mercury ions bind specifically at thymine-thymine mismatches within self-hybridized single-stranded DNA, enabling precise control over the number and position of Hg2+ along the helical axis. Differential charging of the organic layers, manifested as substrate-magnetization-dependent photoionization energies, was observed for DNA hairpins containing Hg2+; no differences were measured for hairpin monolayers in the absence of Hg2+. Inversion of the DNA helical secondary structure at increased metal loading led to complementary inversion in spin selectivity. We attribute these results to increased scattering probabilities from relativistic enhancement of spin-orbit interactions in mercurated DNA.
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