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<p>Electrically probing the spin state of localized <i>f</i> electrons in a rare-earth-based single-molecule magnet, along with understanding its intramolecular magnetic coupling, is of crucial importance for applications in quantum information and advanced spintronics, yet it remains experimentally challenging. Herein, within a single-molecule magnet terbium(III) bis(phthalocyaninato) (TbPc<sub>2</sub>) double-decker molecule adsorbed on a bilayer graphene epitaxially grown on a SiC(0001) substrate, we experimentally demonstrate a spatially dependent exchange interaction between the magnetic moment of the localized Tb 4<i>f</i> electron and the unpaired spin of the Pc <i>π</i>-radical. The magnetic state of TbPc<sub>2</sub>, associated with the <i>f</i>-<i>π</i> interaction, is evidently detected through the spectroscopic Kondo resonance and a zero-field Kondo splitting, which can be reversibly switched in a charge/discharge process triggered by the tip-molecule distance. Furthermore, we theoretically describe how the Kondo resonance evolves at the molecular scale, which is mediated by the <i>f</i>-<i>π</i> exchange interaction with its strength varying spatially in a radial decay fashion. Our spatially resolved Kondo characteristics offer a quantitative understanding of the many-body spin correlation, which is coupled with the charge states in a nonuniform and spatially extended system.</p>

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Spatially dependent f-π exchange interaction within a single-molecule magnet TbPc2

  • 期刊论文

  • 出版模式：

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  • 发表日期：

    2025年7月7日

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  • Xin Liao,
  • Yun Chen,
  • Tao Xie,
  • Rui-Jing Sun,
  • Lian-Zhi Yang,
  • Chao-Fei Liu,
  • Rui Wang,
  • Svetlana Klyatskaya,
  • Mario Ruben,
  • Wenhao Zhang,
  • Ying-Shuang Fu

摘要

Electrically probing the spin state of localized f electrons in a rare-earth-based single-molecule magnet, along with understanding its intramolecular magnetic coupling, is of crucial importance for applications in quantum information and advanced spintronics, yet it remains experimentally challenging. Herein, within a single-molecule magnet terbium(III) bis(phthalocyaninato) (TbPc2) double-decker molecule adsorbed on a bilayer graphene epitaxially grown on a SiC(0001) substrate, we experimentally demonstrate a spatially dependent exchange interaction between the magnetic moment of the localized Tb 4f electron and the unpaired spin of the Pc π-radical. The magnetic state of TbPc2, associated with the f-π interaction, is evidently detected through the spectroscopic Kondo resonance and a zero-field Kondo splitting, which can be reversibly switched in a charge/discharge process triggered by the tip-molecule distance. Furthermore, we theoretically describe how the Kondo resonance evolves at the molecular scale, which is mediated by the f-π exchange interaction with its strength varying spatially in a radial decay fashion. Our spatially resolved Kondo characteristics offer a quantitative understanding of the many-body spin correlation, which is coupled with the charge states in a nonuniform and spatially extended system.