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| Main Authors: | , , |
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| Format: | Preprint |
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2026
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| Online Access: | https://arxiv.org/abs/2603.22725 |
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| _version_ | 1866908908933611520 |
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| author | Afugu, Amos Kafle, Gyanu P. Liu, Zhen-Fei |
| author_facet | Afugu, Amos Kafle, Gyanu P. Liu, Zhen-Fei |
| contents | Spin-resolved photoelectron spectroscopy (PES) is a major experimental probe of chirality-induced spin selectivity (CISS), yet it remains unclear whether the measured spin polarization reflects molecular chirality itself or the broader electronic structure of the hybrid interface. We present a first-principles theory of PES spin polarization at chiral molecule-metal interfaces, treating the interface holistically rather than as a metal substrate plus a separate molecular spin filter/polarizer. Using density functional theory within a three-step photoemission framework, we compute the spin polarization generated in the optical-excitation step for ($M$)- and ($P$)-heptahelicene adsorbed on Au(111) and Cu(111), and for coronene/Au(111) as a non-chiral control. We find that adsorption strongly reshapes the PES spin polarization relative to the clean metal surface, but opposite enantiomers yield symmetry-related, qualitatively similar responses that are also comparable to that of the non-chiral coronene. These results indicate that changes in the PES spin polarization are more naturally attributed to the electronic structure of the hybrid interface than to molecular chirality alone. |
| format | Preprint |
| id |
arxiv_https___arxiv_org_abs_2603_22725 |
| institution | arXiv |
| publishDate | 2026 |
| record_format | arxiv |
| spellingShingle | First-Principles Theory of Chirality-Induced Spin Selectivity at Molecule-Metal Interfaces in Photoemission Afugu, Amos Kafle, Gyanu P. Liu, Zhen-Fei Materials Science Spin-resolved photoelectron spectroscopy (PES) is a major experimental probe of chirality-induced spin selectivity (CISS), yet it remains unclear whether the measured spin polarization reflects molecular chirality itself or the broader electronic structure of the hybrid interface. We present a first-principles theory of PES spin polarization at chiral molecule-metal interfaces, treating the interface holistically rather than as a metal substrate plus a separate molecular spin filter/polarizer. Using density functional theory within a three-step photoemission framework, we compute the spin polarization generated in the optical-excitation step for ($M$)- and ($P$)-heptahelicene adsorbed on Au(111) and Cu(111), and for coronene/Au(111) as a non-chiral control. We find that adsorption strongly reshapes the PES spin polarization relative to the clean metal surface, but opposite enantiomers yield symmetry-related, qualitatively similar responses that are also comparable to that of the non-chiral coronene. These results indicate that changes in the PES spin polarization are more naturally attributed to the electronic structure of the hybrid interface than to molecular chirality alone. |
| title | First-Principles Theory of Chirality-Induced Spin Selectivity at Molecule-Metal Interfaces in Photoemission |
| topic | Materials Science |
| url | https://arxiv.org/abs/2603.22725 |