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Imaging Grains and Grain Boundaries in Single-Layer Graphene: An Atomic Patchwork Quilt  [PDF]
Pinshane Y. Huang,Carlos S. Ruiz-Vargas,Arend M. van der Zande,William S. Whitney,Shivank Garg,Jonathan S. Alden,Caleb J. Hustedt,Ye Zhu,Jiwoong Park,Paul L. McEuen,David A. Muller
Physics , 2010, DOI: 10.1038/nature09718
Abstract: The properties of polycrystalline materials are often dominated by the size of their grains and by the atomic structure of their grain boundaries. These effects should be especially pronounced in 2D materials, where even a line defect can divide and disrupt a crystal. These issues take on practical significance in graphene, a hexagonal two-dimensional crystal of carbon atoms; Single-atom-thick graphene sheets can now be produced by chemical vapor deposition on up to meter scales, making their polycrystallinity almost unavoidable. Theoretically, graphene grain boundaries are predicted to have distinct electronic, magnetic, chemical, and mechanical properties which strongly depend on their atomic arrangement. Yet, because of the five-order-of-magnitude size difference between grains and the atoms at grain boundaries, few experiments have fully explored the graphene grain structure. Here, we use a combination of old and new transmission electron microscope techniques to bridge these length scales. Using atomic-resolution imaging, we determine the location and identity of every atom at a grain boundary and find that different grains stitch together predominantly via pentagon-heptagon pairs. We then use diffraction-filtered imaging to rapidly map the location, orientation, and shape of several hundred grains and boundaries, where only a handful have been previously reported. The resulting images reveal an unexpectedly small and intricate patchwork of grains connected by tilt boundaries. By correlating grain imaging with scanned probe measurements, we show that these grain boundaries dramatically weaken the mechanical strength of graphene membranes, but do not measurably alter their electrical properties. These techniques open a new window for studies on the structure, properties, and control of grains and grain boundaries in graphene and other 2D materials.
Atomic-scale electron-beam sculpting of defect-free graphene nanostructures  [PDF]
Bo Song,Grégory F. Schneider,Qiang Xu,Grégory Pandraud,Cees Dekker,Henny Zandbergen
Physics , 2011, DOI: 10.1021/nl200369r
Abstract: In order to harvest the many promising properties of graphene in (electronic) applications, a technique is required to cut, shape or sculpt the material on a nanoscale without damage to its atomic structure, as this drastically influences the electronic properties of the nanostructure. Here, we reveal a temperature-dependent self-repair mechanism allowing damage-free atomic-scale sculpting of graphene using a focused electron beam. We demonstrate that by sculpting at temperatures above 600 {\deg}C, an intrinsic self-repair mechanism keeps the graphene single-crystalline during cutting, even thought the electron beam induces considerable damage. Self-repair is mediated by mobile carbon ad-atoms constantly repairing the defects caused by the electron beam. Our technique allows reproducible fabrication and simultaneous imaging of single-crystalline free-standing nanoribbons, nanotubes, nanopores, and single carbon chains.
Selective metal deposition at graphene line defects by atomic layer deposition  [PDF]
Kwanpyo Kim,Han-Bo-Ram Lee,Richard W. Johnson,Jukka T. Tanskanen,Nan Liu,Myung-Gil Kim,Changhyun Pang,Chiyui Ahn,Stacey F. Bent,Zhenan Bao
Physics , 2014, DOI: 10.1038/ncomms5781
Abstract: One-dimensional defects in graphene have strong influence on its physical properties, such as electrical charge transport and mechanical strength. With enhanced chemical reactivity, such defects may also allow us to selectively functionalize the material and systematically tune the properties of graphene. Here we demonstrate the selective deposition of metal at chemical vapour deposited graphene's line defects, notably grain boundaries, by atomic layer deposition. Atomic layer deposition allows us to deposit Pt predominantly on graphene's grain boundaries, folds, and cracks due to the enhanced chemical reactivity of these line defects, which is directly confirmed by transmission electron microscopy imaging. The selective functionalization of graphene defect sites, together with the nanowire morphology of deposited Pt, yields a superior platform for sensing applications. Using Pt-graphene hybrid structures, we demonstrate high-performance hydrogen gas sensors at room temperatures and show its advantages over other evaporative Pt deposition methods, in which Pt decorates graphene surface non-selectively.
Direct Imaging of Graphene Edges: Atomic Structure and Electronic Scattering  [PDF]
Jifa Tian,Helin Cao,Wei Wu,Qingkai Yu,Yong P. Chen
Physics , 2011, DOI: 10.1021/nl201590f
Abstract: We report an atomically-resolved scanning tunneling microscopy (STM) investigation of the edges of graphene grains synthesized on Cu foils by chemical vapor deposition (CVD). Most of the edges are macroscopically parallel to the zigzag directions of graphene lattice. These edges have microscopic roughness that is found to also follow zigzag directions at atomic scale, displaying many ~120 degree turns. A prominent standing wave pattern with periodicity ~3a/4 (a being the graphene lattice constant) is observed near a rare-occurring armchair-oriented edge. Observed features of this wave pattern are consistent with the electronic intervalley backscattering predicted to occur at armchair edges but not at zigzag edges.
Atomic resolution imaging of the two-component Dirac-Landau levels in a gapped graphene monolayer  [PDF]
Wen-Xiao Wang,Long-Jing Yin,Jia-Bin Qiao,Tuocheng Cai,Si-Yu Li,Rui-Fen Dou,Jia-Cai Nie,Xiaosong Wu,Lin He
Physics , 2015, DOI: 10.1103/PhysRevB.92.165420
Abstract: The wavefunction of massless Dirac fermions is a two-component spinor. In graphene, a one-atom-thick film showing two-dimensional Dirac-like electronic excitations, the two-component representation reflects the amplitude of the electron wavefunction on the A and B sublattices. This unique property provides unprecedented opportunities to image the two components of massless Dirac fermions spatially. Here we report atomic resolution imaging of the two-component Dirac-Landau levels in a gapped graphene monolayer by scanning tunnelling microscopy and spectroscopy. A gap of about 20 meV, driven by inversion symmetry breaking by the substrate potential, is observed in the graphene on both SiC and graphite substrates. Such a gap splits the n = 0 Landau level (LL) into two levels, 0+ and 0-. We demonstrate that the amplitude of the wavefunction of the 0- LL is mainly at the A sites and that of the 0+ LL is mainly at the B sites of graphene, characterizing the internal structure of the spinor of the n = 0 LL. This provides direct evidence of the two-component nature of massless Dirac fermions.
Tuning the electronic structure of graphene by ion irradiation  [PDF]
Levente Tapaszto,Gergely Dobrik,Peter Nemes-Incze,Gabor Vertesy,Philippe Lambin,Laszlo P Biro
Physics , 2009, DOI: 10.1103/PhysRevB.78.233407
Abstract: Mechanically exfoliated graphene layers deposited on SiO2 substrate were irradiated with Ar+ ions in order to experimentally study the effect of atomic scale defects and disorder on the low-energy electronic structure of graphene. The irradiated samples were investigated by scanning tunneling microscopy and spectroscopy measurements, which reveal that defect sites, besides acting as scattering centers for electrons through local modification of the on-site potential, also induce disorder in the hopping amplitudes. The most important consequence of the induced disorder is the substantial reduction in the Fermi velocity, revealed by bias-dependent imaging of electron-density oscillations observed near defect sites.
Native defects in ultra-high vacuum grown graphene islands on Cu(111)  [PDF]
S. M. Hollen,S. J. Tjung,K. R. Mattioli,G. A. Gambrel,N. M. Santagata,E. Johnston-Halperin,J. A. Gupta
Physics , 2015,
Abstract: We present a scanning tunneling microscopy (STM) study of native defects in graphene islands grown by ultra-high vacuum (UHV) decomposition of ethylene on Cu(111). We characterize these defects through a survey of their apparent heights, atomic-resolution imaging, and detailed tunneling spectroscopy. Bright defects that occur only in graphene regions are identified as C site point defects in the graphene lattice and are most likely single C vacancies. Dark defect types are observed in both graphene and Cu regions, and are likely point defects in the Cu surface. We also present data showing the importance of bias and tip termination to the appearance of the defects in STM images and the ability to achieve atomic resolution. Finally, we present tunneling spectroscopy measurements probing the influence of point defects on the local electronic landscape of graphene islands.
Electronic and structural characterization of divacancies in irradiated graphene  [PDF]
Miguel M. Ugeda,Iván Brihuega,Fanny Hiebel,Pierre Mallet,Jean-Yves Veuillen,José M. Gómez-Rodríguez,Félix Ynduráin
Physics , 2011, DOI: 10.1103/PhysRevB.85.121402
Abstract: We provide a thorough study of a carbon divacancy, a fundamental but almost unexplored point defect in graphene. Low temperature scanning tunneling microscopy (STM) imaging of irradiated graphene on different substrates enabled us to identify a common two-fold symmetry point defect. Our first principles calculations reveal that the structure of this type of defect accommodates two adjacent missing atoms in a rearranged atomic network formed by two pentagons and one octagon, with no dangling bonds. Scanning tunneling spectroscopy (STS) measurements on divacancies generated in nearly ideal graphene show an electronic spectrum dominated by an empty-states resonance, which is ascribed to a spin-degenerated nearly flat band of $\pi$-electron nature. While the calculated electronic structure rules out the formation of a magnetic moment around the divacancy, the generation of an electronic resonance near the Fermi level, reveals divacancies as key point defects for tuning electron transport properties in graphene systems.
Atomic Layer Deposition of Metal Oxides on Pristine and Functionalized Graphene  [PDF]
Xinran Wang,Scott Tabakman,Hongjie Dai
Physics , 2008,
Abstract: We investigate Atomic Layer Deposition (ALD) of metal oxide on pristine and functionalized graphene. On pristine graphene, ALD coating can only actively grow on edges and defect sites, where dangling bonds or surface groups react with ALD precursors. This affords a simple method to decorate and probe single defect sites in graphene planes. We used perylene tetracarboxylic acid (PTCA) to functionalize graphene surface and selectively introduced densely packed surface groups on graphene. Uniform ultrathin ALD coating on PTCA graphene was achieved over large area. The functionalization method could be used to integrate ultrathin high-k dielectrics in future graphene electronics.
Seebeck effect at the atomic scale  [PDF]
Eui-Sup Lee,Sanghee Cho,Ho-Ki Lyeo,Yong-Hyun Kim
Physics , 2013, DOI: 10.1103/PhysRevLett.112.136601
Abstract: The atomic variations of electronic wavefunctions at the surface and electron scattering near a defect have been detected unprecedentedly by tracing thermoelectric voltages given a temperature bias [Cho et al., Nature Mater. 12, 913 (2013)]. Because thermoelectricity, or Seebeck effect, is associated with heat-induced electron diffusion, how the thermoelectric signal is related to the atomic-scale wavefunctions and what the role of the temperature is at such a length scale remain very unclear. Here we show that coherent electron and heat transport through a point-like contact produces an atomic Seebeck effect, which is described by mesoscopic Seebeck coefficient multiplied with an effective temperature drop at the interface. The mesoscopic Seebeck coefficient is approximately proportional to the logarithmic energy derivative of local density of states at the Fermi energy. We deduced that the effective temperature drop at the tip-sample junction could vary at a sub-angstrom scale depending on atom-to-atom interaction at the interface. A computer-based simulation method of thermoelectric images is proposed, and a point defect in graphene was identified by comparing experiment and the simulation of thermoelectric imaging.
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