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Abstract Carbon‐based quantum dots (QDs) enable flexible manipulation of electronic behavior at the nanoscale, but controlling their magnetic properties requires atomically precise structural control. While magnetism is observed in organic molecules and graphene nanoribbons (GNRs), GNR precursors enabling bottom‐up fabrication of QDs with various spin ground states have not yet been reported. Here the development of a new GNR precursor that results in magnetic QD structures embedded in semiconducting GNRs is reported. Inserting one such molecule into the GNR backbone and graphitizing it results in a QD region hosting one unpaired electron. QDs composed of two precursor molecules exhibit nonmagnetic, antiferromagnetic, or antiferromagnetic ground states, depending on the structural details that determine the coupling behavior of the spins originating from each molecule. The synthesis of these QDs and the emergence of localized states are demonstrated through high‐resolution atomic force microscopy (HR‐AFM), scanning tunneling microscopy (STM) imaging, and spectroscopy, and the relationship between QD atomic structure and magnetic properties is uncovered. GNR QDs provide a useful platform for controlling the spin‐degree of freedom in carbon‐based nanostructures.
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Tuning interactions between spins in a superconductor
Novel many-body and topological electronic phases can be created in assemblies of interacting spins coupled to a superconductor, such as one-dimensional topological superconductors with Majorana zero modes (MZMs) at their ends. Understanding and controlling interactions between spins and the emergent band structure of the in-gap Yu–Shiba–Rusinov (YSR) states they induce in a superconductor are fundamental for engineering such phases. Here, by precisely positioning magnetic adatoms with a scanning tunneling microscope (STM), we demonstrate both the tunability of exchange interaction between spins and precise control of the hybridization of YSR states they induce on the surface of a bismuth (Bi) thin film that is made superconducting with the proximity effect. In this platform, depending on the separation of spins, the interplay among Ruderman–Kittel–Kasuya–Yosida (RKKY) interaction, spin–orbit coupling, and surface magnetic anisotropy stabilizes different types of spin alignments. Using high-resolution STM spectroscopy at millikelvin temperatures, we probe these spin alignments through monitoring the spin-induced YSR states and their energy splitting. Such measurements also reveal a quantum phase transition between the ground states with different electron number parity for a pair of spins in a superconductor tuned by their separation. Experiments on larger assemblies show that spin–spin interactions can be mediated in a superconductor over long distances. Our results show that controlling hybridization of the YSR states in this platform provides the possibility of engineering the band structure of such states for creating topological phases.
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- PAR ID:
- 10219316
- Publisher / Repository:
- Proceedings of the National Academy of Sciences
- Date Published:
- Journal Name:
- Proceedings of the National Academy of Sciences
- Volume:
- 118
- Issue:
- 14
- ISSN:
- 0027-8424
- Page Range / eLocation ID:
- Article No. e2024837118
- Format(s):
- Medium: X
- Sponsoring Org:
- National Science Foundation
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