A combination of angle-resolved photoemission and scanning tunneling microscopy is used to explore the possibilities for tailoring the electronic structure of gold atom chains on silicon surfaces. It is shown that the interchain coupling and the band filling can be adjusted systematically by varying the step spacing via the tilt angle from Si͑111͒. Planes with odd Miller indices are stabilized by chains of gold atoms. Metallic bands and Fermi surfaces are observed. These findings suggest that atomic chains at stepped semiconductor substrates make a highly flexible class of solids approaching the one-dimensional limit.
We report the synthesis of extended two-dimensional organic networks on Cu(111), Ag(111), Cu(110), and Ag(110) from thiophene-based molecules. A combination of scanning tunnelling microscopy and X-ray photoemission spectroscopy yields insight into the reaction pathways from single molecules towards the formation of two-dimensional organometallic and polymeric structures via Ullmann reaction dehalogenation and C-C coupling. The thermal stability of the molecular networks is probed by annealing at elevated temperatures of up to 500 °C. On Cu(111) only organometallic structures are formed, while on Ag(111) both organometallic and covalent polymeric networks were found to coexist. The ratio between organometallic and covalent bonds could be controlled by means of the annealing temperature. The thiophene moieties start degrading at 200 °C on the copper surface, whereas on silver the degradation process becomes significant only at 400 °C. Our work reveals how the interplay of a specific surface type and temperature steers the formation of organometallic and polymeric networks and describes how these factors influence the structural integrity of two-dimensional organic networks.
The Si͑111͒5 ϫ 2-Au surface exhibits a chain structure with additional Si atoms on top of the chains. They dope the chains to achieve the optimum band filling, according to recent local density calculations. Surprisingly, the Si atoms form a half-filled, disordered 5 ϫ 4 lattice fluid, not an ordered 5 ϫ 8 lattice. From their autocorrelation function an interatomic potential with 5 ϫ 4 periodicity was deduced. An explanation for the 5 ϫ 4 periodicity is provided by establishing a connection to the electronic structure near the Fermi level E F , which is mapped by angle-resolved photoemission. The constant energy surfaces near E F consist of onedimensional lines at the boundaries of a 5 ϫ 4 Brillouin zone. Such nested features of high density of states are capable of triggering a 5 ϫ 4 superlattice interaction. The measurements establish a two-way connection between electronic structure and interatomic potentials: A one-dimensional Fermi surface instability triggers a superlattice of extra atoms, and the atoms provide the correct number of electrons for such an instability to occur. The band structure is discussed in view of the recently observed phase-separation into nanometer-sized segments of metallic and semiconducting character.
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