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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Comprehensive Electrostatic Modeling of Exposed Quantum Dots in Graphene/Hexagonal Boron Nitride Heterostructures
Recent experimental advancements have enabled the creation of tunable localized electrostatic potentials in graphene/hexagonal boron nitride (hBN) heterostructures without concealing the graphene surface. These potentials corral graphene electrons yielding systems akin to electrostatically defined quantum dots (QDs). The spectroscopic characterization of these exposed QDs with the scanning tunneling microscope (STM) revealed intriguing resonances that are consistent with a tunneling probability of 100% across the QD walls. This effect, known as Klein tunneling, is emblematic of relativistic particles, underscoring the uniqueness of these graphene QDs. Despite the advancements with electrostatically defined graphene QDs, a complete understanding of their spectroscopic features still remains elusive. In this study, we address this lapse in knowledge by comprehensively considering the electrostatic environment of exposed graphene QDs. We then implement these considerations into tight binding calculations to enable simulations of the graphene QD local density of states. We find that the inclusion of the STM tip’s electrostatics in conjunction with that of the underlying hBN charges reproduces all of the experimentally resolved spectroscopic features. Our work provides an effective approach for modeling the electrostatics of exposed graphene QDs. The methods discussed here can be applied to other electrostatically defined QD systems that are also exposed.
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- Award ID(s):
- 1753367
- PAR ID:
- 10222485
- Date Published:
- Journal Name:
- Nanomaterials
- Volume:
- 10
- Issue:
- 6
- ISSN:
- 2079-4991
- Page Range / eLocation ID:
- 1154
- Format(s):
- Medium: X
- Sponsoring Org:
- National Science Foundation
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