Protection of excited spin states by a superconducting energy gap

The latest concepts for quantum computing and data storage envision to address and manipulate single spins. A limitation for single atoms or molecules in contact to a metal surface are the short lifetime of excited spin states, typically picoseconds, due to the exchange of energy and angular momentum with the itinerant electrons of the substrate [1-4]. Here we show that paramagnetic molecules on a superconducting substrate exhibit excited spin states with a lifetime of approximately 10 ns. We ascribe this increase in lifetime by orders of magnitude to the depletion of electronic states within the energy gap at the Fermi level. This prohibits pathways of energy relaxation into the substrate and allows for electrically pumping the magnetic molecule into higher spin states, making superconducting substrates premium candidates for spin manipulation. We further show that the proximity of the scanning tunneling microscope tip modifies the magnetic anisotropy.

Engineering Negative Differential Conductance with the Cu(111) Surface State

Low-temperature scanning tunneling microscopy and spectroscopy are employed to investigate electron tunneling from a C60-terminated tip into a Cu(111) surface. Tunneling between a C60 orbital and the Shockley surface states of copper is shown to produce negative differential conductance (NDC) contrary to conventional expectations. NDC can be tuned through barrier thickness or C60 orientation up to complete extinction. The orientation dependence of NDC is a result of a symmetry matching between the molecular tip and the surface states.

Visualizing the spin of individual molecules

Low-temperature spin-polarized scanning tunneling microscopy is employed to study spin transport across single Cobalt-Phathalocyanine molecules adsorbed on well characterized magnetic nanoleads. A spin-polarized electronic resonance is identified over the center of the molecule and exploited to spatially resolve stationary spin states. These states reflect two molecular spin orientations and, as established by density functional calculations, originate from a ferromagnetic molecule-lead superexchange interaction mediated by the organic ligands.