Bilayer of Terbium Double-Decker Single-Molecule Magnets

[Image: see text] We report a low-temperature scanning tunneling microscopy and spectroscopy study of the structural and electronic properties of a bilayer of terbium double-decker (bis(phthalocyaninato)terbium(III), TbPc(2)) molecules on Au(111) at 5 K. The TbPc(2) molecules are found to adsorb flat on top of a first compact TbPc(2) monolayer on Au(111), forming a square-like packing similar to the underlying first layer. Their frontier-orbital electronic structure, measured by tunneling conductance spectroscopy, clearly differs from that of the underlying first monolayer. Our results of second-layer molecules indicate the absence of, both, hybrid molecule–substrate electronic states close to the Fermi level and a zero-bias Kondo resonance. We attribute these findings to a decreased electronic coupling with the Au(111) substrate.