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arXiv · 1805.03913

On-Surface Structural and Electronic Properties of Spontaneously Formed Tb$_2$Pc$_3$ Single Molecule Magnets

Jack Hellerstedt·Aleš Cahlík·Martin Švec·Bruno de la Torre·María Moro-Lagares·Barbora Papoušková·Giorgio Zoppellaro·Pingo Mutombo·Mario Ruben·Radek Zbořil·Pavel Jelinek
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Abstract

The single molecule magnet (SMM) bis(phthalocyaninato)terbium (III) (TbPc$_2$) has attracted steady research attention as an exemplar system for realizing molecule-based spin electronics. In this paper, we report on the spontaneous formation of Tb$_2$Pc$_3$ species from TbPc$_2$ precursors via sublimation in ultrahigh vacuum (UHV) onto an Ag(111) surface. The molecules on the surface are inspected using combined scanning tunneling (STM) and non-contact atomic force microscopies (nc-AFM) at 5 Kelvin. Submolecular resolution and height dependent measurements supported by density functional theory (DFT) calculations unambiguously show the presence of both TbPc$_2$ and Tb$_2$Pc$_3$ species. The synthesis of Tb$_2$Pc$_3$ species under UHV conditions is independently confirmed by chemical analysis. The high-resolution AFM imaging allows us to register the orientation of the topmost Pc ligand in both Tb$_2$Pc$_3$ and TbPc$_2$ relative to the underlying Ag(111) surface. Measurements of the electronic structure reveal the selective appearance of a Kondo signature with temperature $\sim$ 30K in the Tb$_2$Pc$_3$ species, localized to the Pc ligand lobes. We attribute the presence of the Kondo resonance on select Tb$_2$Pc$_3$ molecules to the orientation of internal molecular ligands. High-resolution AFM imaging identifies geometric distortions between Tb$_2$Pc$_3$ molecules with and without the Kondo effect, the result of the complex interplay between structural and electronic differences.

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Jack Hellerstedt, Aleš Cahlík, Martin Švec, Bruno de la Torre, María Moro-Lagares, Barbora Papoušková, Giorgio Zoppellaro, Pingo Mutombo, Mario Ruben, Radek Zbořil, Pavel Jelinek. 2018-05-10. On-Surface Structural and Electronic Properties of Spontaneously Formed Tb$_2$Pc$_3$ Single Molecule Magnets. https://doi.org/10.1039/c8nr04215b

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