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Bibliographic Details
Main Authors: Baljozović, Miloš, Karmakar, Shiladitya, Cauduro, André L. Fernandes, Sundar, Mothuku Shyam, Lozano, Marco, Kumar, Manish, Polo, Diego Soler, Schmid, Andreas K., Bedekar, Ashutosh V., Jelinek, Pavel, Ernst, Karl-Heinz
Format: Preprint
Published: 2025
Subjects:
Online Access:https://arxiv.org/abs/2510.03897
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Table of Contents:
  • We report the emergence of adsorption-induced magnetism from heterohelicene molecules on a non-magnetic Cu(100) surface. Spin-polarized low-energy electron microscopy (SP-LEEM) measurements reveal spin-dependent electron reflectivity for enantiopure 7,12,17-trioxa[11]helicene (TO[11]H) monolayers, indicating the formation of a spin-polarized state localized in the topmost copper layer. Control experiments on clean Cu(100) and TO[11]H on highly oriented pyrolytic graphite show no such effect, excluding artifacts and chirality-induced spin selectivity as origins. Spin-polarized density functional theory calculations with hybrid functionals attribute the magnetism to strong chemisorption, which induces hybridization between the molecular HOMO and copper s- and d-states, driving asymmetric spin-polarized charge redistribution at the interface. An extended Newns-Anderson-Grimley model incorporating on-site Coulomb repulsion in Cu d-orbitals reproduces the emergence of interfacial spin polarization above a threshold interaction strength, highlighting the key roles of hybridization parameters and Coulomb correlation. These findings reveal a mechanism for inducing magnetism at molecule-metal interfaces without inherently magnetic components, offering avenues for engineering spin-polarized states in organic-inorganic hybrid systems.