Publications

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We use low-energy electron microscopy to investigate how graphene is removed from Ru(0001) and Ir(111) by reaction with oxygen. We find two mechanisms on Ru(0001). At short times, oxygen reacts with carbon monomers on the surrounding Ru surface, decreasing their concentration below the equilibrium value. This undersaturation causes a flux of carbon from graphene to the monomer gas. In this initial mechanism, graphene is etched at a rate that is given precisely by the same nonlinear dependence on carbon monomer concentration that governs growth. Thus, during both growth and etching, carbon attaches and detaches to graphene as clusters of several carbon atoms. At later times, etching accelerates. We present evidence that this process involves intercalated oxygen, which destabilizes graphene. On Ir, this mechanism creates observable holes. It also occurs mostly quickly near wrinkles in the graphene islands, depends on the orientation of the graphene with respect to the Ir substrate, and, in contrast to the first mechanism, can increase the density of carbon monomers. We also observe that both layers of bilayer graphene islands on Ir etch together, not sequentially. © 2010 American Chemical Society.

Growth of high quality graphene films on SiC is regarded as one of the more viable pathways toward graphene-based electronics. Graphitic films form on SiC at elevated temperature because of preferential sublimation of Si. Little is known, however, about the atomistic processes of interrelated SiC decomposition and graphene growth. We have observed the formation of graphene on SiC by Si sublimation in an Ar atmosphere using low energy electron microscopy, scanning tunneling microcopy and atomic force microscopy. This work reveals that the growth mechanism depends strongly on the initial surface morphology, and that carbon diffusion governs the spatial relationship between SiC decomposition and graphene growth. Isolated bilayer SiC steps generate narrow ribbons of graphene, whereas triple bilayer steps allow large graphene sheets to grow by step flow. We demonstrate how graphene quality can be improved by controlling the initial surface morphology specifically by avoiding the instabilities inherent in diffusion-limited growth.

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We study how single-crystal chromium films of uniform thickness on W(110) substrates are converted to arrays of three-dimensional (3D) Cr islands during annealing. We use low-energy electron microscopy (LEEM) to directly observe a kinetic pathway that produces trenches that expose the wetting layer. Adjacent film steps move simultaneously uphill and downhill relative to the staircase of atomic steps on the substrate. This step motion thickens the film regions where steps advance. Where film steps retract, the film thins, eventually exposing the stable wetting layer. Since our analysis shows that thick Cr films have a lattice constant close to bulk Cr, we propose that surface and interface stress provide a possible driving force for the observed morphological instability. Atomistic simulations and analytic elastic models show that surface and interface stress can cause a dependence of film energy on thickness that leads to an instability to simultaneous thinning and thickening. We observe that de-wetting is also initiated at bunches of substrate steps in two other systems, Ag/W(110) and Ag/Ru(0001). We additionally describe how Cr films are converted into patterns of unidirectional stripes as the trenches that expose the wetting layer lengthen along the W[001] direction. Finally, we observe how 3D Cr islands. © IOP Publishing Ltd and Deutsche Physikalische Gesellschaft.

We have studied the dislocation structures that occur in films of Ag, Au, and Ag{sub 0.5}Au{sub 0.5} alloy on a Ru(0001) substrate. Monolayer (ML) films form herringbone phases while films two or more layers thick contain triangular patterns of dislocations. We use scanning tunneling microscopy (STM) and low-energy electron diffraction (LEED) to determine how the film composition affects the structure and periodicity of these ordered structures. One layer of Ag forms two different herringbone phases depending on the exact Ag coverage and temperature. Low-energy electron microscopy (LEEM) establishes that a reversible, first-order phase transition occurs between these two phases at a certain temperature. We critically compare our 1 ML Ag structures to conflicting results from an X-ray scattering study [H. Zajonz et al., Phys. Rev. B 67 (2003) 155417]. Unlike Ag, the herringbone phases of Au and AgAu alloy are independent of the exact film coverage. For two layer films in all three systems, none of the dislocations in the triangular networks thread into the second film layer. In all three systems, the in-plane atomic spacing of the second film layer is nearly the same as in the bulk. Film composition does, however, affect the details of the two layer structures. Ag and Au films form interconnected networks of dislocations, which we refer to as 'trigons.' In 2 ML AgAu alloy, the dislocations form a different triangular network that shares features of both trigon and moire structures. Yet another well-ordered structure, with square symmetry, forms at the boundaries of translational trigon domains in 2 ML Ag films but not in Au films.

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We track individual twin boundaries in Ag films on Ru(0001) using low-energy electron microscopy. The twin boundaries, which separate film regions whose close-packed planes are stacked differently, move readily during film growth but relatively little during annealing. The growth-driven motion of twin boundaries occurs as film steps advance across the surface-as a new atomic Ag layer reaches an fcc twin boundary, the advancing step edge carries along the boundary. This coupling of the microstructural defect (twin boundary) and the surface step during growth can produce film regions over 10μm wide that are twin free. © 2005 The American Physical Society.

We have used scanning tunneling microscopy and low-energy electron microscopy to measure the thermal decay of two-dimensional Cu, Pb-overlayer, and Pb-Cu alloy islands on Pb-Cu(1 1 1) surface alloys. Decay rates covering 6-7 orders of magnitude are accessible by applying the two techniques to the same system. We find that Cu adatom diffusion across the surface alloy is rate-limiting for the decay of both Pb and Pb-Cu islands on the surface alloy and that this rate decreases monotonically with increasing Pb concentration in the alloy. The decrease is attributed to repulsive interactions between Cu adatoms and embedded Pb atoms in the surface alloy. The measured temperature dependences of island decay rates are consistent with first-principles calculations of the Cu binding and diffusion energies related to this 'site-blocking' effect.

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We find that small temperature changes cause steps on the NiAl(110) surface to move. We show that this step motion occurs because mass is transferred between the bulk and the surface as the concentration of bulk thermal defects (i.e., vacancies) changes with temperature. Since the change in an island's area with a temperature change is found to scale strictly with the island's step length, the thermally generated defects are created (annihilated) very near the surface steps. To quantify the bulk/surface exchange, we oscillate the sample temperature and measure the amplitude and phase lag of the system response, i.e., the change in an island's area normalized to its perimeter. Using a one-dimensional model of defect diffusion through the bulk in a direction perpendicular to the surface, we determine the migration and formation energies of the bulk thermal defects. During surface smoothing, we show that there is no flow of material between islands on the same terrace and that all islands in a stack shrink at the same rate. We conclude that smoothing occurs by mass transport through the bulk of the crystal rather than via surface diffusion. Based on the measured relative sizes of the activation energies for island decay, defect migration, and defect formation, we show that attachment/detachment at the steps is the rate-limiting step in smoothing.