Abstract2D sheets of graphene‐like silicon, namely planar silicene, are synthesized. This new silicon allotrope is prepared on Au(111) thin films grown on a Si(111) substrate in the process of surface segregation. Owing to its almost perfectly flat geometry it shares the atomic structure with graphene rather than with low‐buckled silicene. Scanning tunneling microscopy measurements clearly display an atomically resolved planar silicene honeycomb lattice. Ab initio density functional theory calculations fully support the experimental findings and predict a pure sp2 atomic configuration of Si atoms. The present work is the first experimental evidence of epitaxial planar silicene.

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The spin-dependent reflectivity of electrons with energies between 0 and 20 eV from Fe single crystals 2-8 monolayers thick on a W(110) surface is studied by spin-polarized low energy electron microscopy. The quantum size oscillations in the reflectivity are analyzed in a similar manner as in photoemission of ground state electrons, yielding the spin-resolved unoccupied state band structure of Fe in the Gamma N direction in the energy range studied.

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