E02-JEM ARM 300CF
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Diamond Proposal Number(s):
[22549]
Abstract: Simultaneous imaging of individual low and high atomic number atoms using annular dark field scanning transmission electron microscopy (ADF-STEM) is often challenging due to substantial differences in their scattering cross sections. This often leads to contrast from only the high atomic number species when imaged using ADF-STEM such as the Mo and 2S sites in monolayer MoS2 crystals, without detection of lighter atoms such as C, O, or N. Here, we show that by capturing an array of convergent beam electron diffraction patterns using a 2D pixelated electron detector (2D-PED) in a 4D STEM geometry enables identification of individual low and high atomic number atoms in 2D materials by multicomponent imaging. We have used ptychographic phase reconstructions, combined with angular dependent ADF-STEM reconstructions, to image light elements at lateral (nanopores) and vertical interfaces (surface dopants) within 2D monolayer MoS2. Differential phase contrast imaging (Div(DPC)) using quadrant segmentation of the 2D pixelated direct electron detector data not only qualitatively matches the ptychographic phase reconstructions in both resolution and contrast but also offers the additional potential for real time display. Using 4D-STEM, we have identified surface adatoms on MoS2 monolayers and have separated atomic columns with similar total atomic number into their relative combinations of low and high atomic number elements. These results demonstrate the rich information present in the data obtained during 4D-STEM imaging of ultrathin 2D materials and the ability of this approach to extract unique insights beyond conventional imaging.
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Aug 2019
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Open Access
Abstract: The properties of nanoparticles are known to critically depend on their local chemistry but characterizing three-dimensional (3D) elemental segregation at the nanometer scale is highly challenging. Scanning transmission electron microscope (STEM) tomographic imaging is one of the few techniques able to measure local chemistry for inorganic nanoparticles but conventional methodologies often fail due to the high electron dose imparted. Here, we demonstrate realization of a new spectroscopic single particle reconstruction approach built on a method developed by structural biologists. We apply this technique to the imaging of PtNi nanocatalysts and find new evidence of a complex inhomogeneous alloying with a Pt-rich core, a Ni-rich hollow octahedral intermediate shell and a Pt-rich rhombic dodecahedral skeleton framework with less Pt at ⟨100⟩ vertices. The ability to gain evidence of local surface enrichment that varies with the crystallographic orientation of facets and vertices is expected to provide significant insight toward the development of nanoparticles for sensing, medical imaging, and catalysis.
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Jan 2019
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I05-ARPES
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Jiagui
Feng
,
Deepnarayan
Biswas
,
Akhil
Rajan
,
Matthew D.
Watson
,
Federico
Mazzola
,
Oliver J.
Clark
,
Kaycee
Underwood
,
I.
Markovic
,
Martin
Mclaren
,
Andrew
Hunter
,
David M.
Burn
,
Liam B.
Duffy
,
Sourabh
Barua
,
Geetha
Balakrishnan
,
Francois
Bertran
,
Patrick
Le Fevre
,
Timur
Kim
,
Gerrit
Van Der Laan
,
Thorsten
Hesjedal
,
Peter
Wahl
,
Phil D. C.
King
Diamond Proposal Number(s):
[19771]
Abstract: How the interacting electronic states and phases of layered transition-metal dichalcogenides
evolve when thinned to the single-layer limit is a key open question in the study of two-dimensional
materials. Here, we use angle-resolved photoemission to investigate the electronic structure of monolayer VSe2 grown on bi-layer graphene/SiC. While the global electronic structure is similar to that of bulk VSe2, we show that, for the monolayer, pronounced energy gaps develop over the entire Fermi surface with decreasing temperature below Tc = 140 5 K, concomitant with the emergence
of charge-order superstructures evident in low-energy electron diffraction. These observations point
to a charge-density wave instability in the monolayer which is strongly enhanced over that of the bulk. Moreover, our measurements of both the electronic structure and of x-ray magnetic circular dichroism reveal no signatures of a ferromagnetic ordering, in contrast to the results of a recent experimental study as well as expectations from density-functional theory. Our study thus points
to a delicate balance that can be realised between competing interacting states and phases in
monolayer transition-metal dichalcogenides.
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Jun 2018
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I09-Surface and Interface Structural Analysis
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Diamond Proposal Number(s):
[15748]
Abstract: Atomically thin two-dimensional (2D) materials exhibit superlative properties dictated by their intralayer atomic structure, which is typically derived from a limited number of thermodynamically stable bulk layered crystals (e.g., graphene from graphite). The growth of entirely synthetic 2D crystals - those with no corresponding bulk allotrope - would circumvent this dependence upon bulk thermodynamics and substantially expand the phase space available for structure-property engineering of 2D materials. However, it remains unclear if synthetic 2D materials can exist as structurally and chemically distinct layers anchored by van der Waals (vdW) forces, as opposed to strongly bound adlayers. Here, we show that atomically thin sheets of boron (i.e., borophene) grown on the Ag(111) surface exhibit a vdW-like structure without a corresponding bulk allotrope. Using X-ray standing wave (XSW)-excited X-ray photoelectron spectroscopy (XPS), the positions of boron in multiple chemical states are resolved with sub-Ångström spatial resolution, revealing that the borophene forms a single planar layer that is 2.4 Å above the unreconstructed Ag surface. Moreover, our results reveal that multiple borophene phases exhibit these characteristics, denoting a unique form of polymorphism consistent with recent predictions. This observation of synthetic borophene as chemically discrete from the growth substrate suggests that it is possible to engineer a much wider variety of 2D materials than those accessible through bulk layered crystal structures.
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Apr 2018
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I06-Nanoscience
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Diamond Proposal Number(s):
[9309]
Abstract: The growth and reactive dewetting of ultra-thin films of iron oxides supported on Re(0001) surfaces have been imaged in-situ in real time. Initial growth forms a non-magnetic stable FeO (wüstite like) layer in a commensurate network upon which high aspect ratio nanowires of several microns length but less than 40nm width can be fabricated. The nanowires are closely aligned with the substrate crystallography and imaging by X-ray magnetic circular dichroism shows that each contain a single magnetic domain. The driving force for dewetting appears to be the minimization of strain energy of the Fe3O4 crystallites and follows the Tersoff and Tromp model in which strain is minimized at constant height by extending in one epitaxially matched direction. Such wires are promising in spintronic applications and we predict that the growth will also occur on other hexagonal substrates.
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Mar 2018
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Abstract: The combination of topological insulators, i.e., bulk insulators with gapless, topologically protected surface states, with magnetic order is a love-hate relationship that can unlock new quantum states and exotic physical phenomena, such as the quantum anomalous Hall effect and axion electrodynamics. Moreover, the unusual coupling between topological insulators and ferromagnets can also result in the formation of topological spin textures in the ferromagnetic layer. Skyrmions are topologically-protected magnetization swirls that are promising candidates for spintronics memory carriers. Here, we report on the observation of skyrmionium in thin ferromagnetic films coupled to a magnetic topological insulator. The occurrence of skyrmionium, which appears as a soliton composed of two skyrmions with opposite winding numbers, is tied to the ferromagnetic state of the topological insulator. Our work presents a new combination of two important classes of topological materials and may open the door to new topologically inspired information-storage concepts in the future.
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Jan 2018
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E02-JEM ARM 300CF
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Diamond Proposal Number(s):
[16856]
Abstract: The edges of 2D materials show novel electronic, magnetic, and optical properties, especially when reduced to nanoribbon widths. Therefore, methods to create atomically flat edges in 2D materials are essential for future exploitation. Atomically flat edges in 2D materials are found after brittle fracture or when electrically biasing, but a simple scalable approach for creating atomically flat periodic edges in monolayer 2D transition metal dichalcogenides has yet to be realized. Here, we show how heating monolayer MoS2 to 800 °C in vacuum produces atomically flat Mo terminated zigzag edges in nanoribbons. We study this at the atomic level using an ultrastable in situ heating holder in an aberration-corrected transmission electron microscope and discriminating Mo from S at the edge, revealing unique Mo terminations for all zigzag orientations that remain stable and atomically flat when cooling back to room temperature. Highly faceted MoS2 nanoribbon constrictions are produced with Mo rich edge structures that have theoretically predicted spin separated transport channels, which are promising for spin logic applications.
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Aug 2017
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I22-Small angle scattering & Diffraction
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Diamond Proposal Number(s):
[14217, 15030, 15530]
Open Access
Abstract: Many emerging technologies require materials with well-defined 3D nanoscale architectures. Production of these structures is currently underpinned by self-assembling amphiphilic macromolecules or engineered all-DNA building blocks. Both these approaches produce restricted ranges of crystal geometries due to synthetic amphiphiles’ simple shape and limited specificity, or the technical difficulties in designing space-filling DNA motifs with targeted shapes. We have overcome these limitations with amphiphilic DNA-nanostructures, or “C-Stars”, that combine the design freedom and facile functionalization of DNA-based materials with robust hydrophobic interactions. C-Stars self-assemble into single crystals exceeding 40 μm in size with lattice parameters exceeding 20 nm.
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Apr 2017
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I05-ARPES
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Diamond Proposal Number(s):
[13946]
Abstract: van der Waals two-dimensional (2D) semiconductors have emerged as a class of materials with promising device characteristics owing to the intrinsic band gap. For realistic applications, the ideal is to modify the band gap in a controlled manner by a mechanism that can be generally applied to this class of materials. Here, we report the observation of a universally tunable band gap in the family of bulk 2H transition metal dichalcogenides (TMDs) by in situ surface doping of Rb atoms. A series of angle-resolved photoemission spectra unexceptionally shows that the band gap of TMDs at the zone corners is modulated in the range of 0.8–2.0 eV, which covers a wide spectral range from visible to near-infrared, with a tendency from indirect to direct band gap. A key clue to understanding the mechanism of this band-gap engineering is provided by the spectroscopic signature of symmetry breaking and resultant spin-splitting, which can be explained by the formation of 2D electric dipole layers within the surface bilayer of TMDs. Our results establish the surface Stark effect as a universal mechanism of band-gap engineering on the basis of the strong 2D nature of van der Waals semiconductors.
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Feb 2017
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I05-ARPES
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Alexander
Generalov
,
Mikhail M.
Otrokov
,
Alla
Chikina
,
Kristin
Kliemt
,
Kurt
Kummer
,
Marc
Höppner
,
Monika
Guttler
,
Silvia
Seiro
,
Alexander
Fedorov
,
Susanne
Schulz
,
Steffen
Danzenbächer
,
Evgueni V.
Chulkov
,
Christoph
Geibel
,
Clemens
Laubschat
,
Pavel
Dudin
,
Moritz
Hoesch
,
Timur
Kim
,
Milan
Radovic
,
Ming
Shi
,
Nicholas C.
Plumb
,
Cornelius
Krellner
,
Denis V.
Vyalikh
Diamond Proposal Number(s):
[11512]
Abstract: Finding ways to create and control the spin-dependent properties of two-dimensional electron states (2DESs) is a major challenge for the elaboration of novel spin-based devices. Spin–orbit and exchange–magnetic interactions (SOI and EMI) are two fundamental mechanisms that enable access to the tunability of spin-dependent properties of carriers. The silicon surface of HoRh2Si2 appears to be a unique model system, where concurrent SOI and EMI can be visualized and controlled by varying the temperature. The beauty and simplicity of this system lie in the 4f moments, which act as a multiple tuning instrument on the 2DESs, as the 4f projections parallel and perpendicular to the surface order at essentially different temperatures. Here we show that the SOI locks the spins of the 2DESs exclusively in the surface plane when the 4f moments are disordered: the Rashba-Bychkov effect. When the temperature is gradually lowered and the system experiences magnetic order, the rising EMI progressively competes with the SOI leading to a fundamental change in the spin-dependent properties of the 2DESs. The spins rotate and reorient toward the out-of-plane Ho 4f moments. Our findings show that the direction of the spins and the spin-splitting of the two-dimensional electrons at the surface can be manipulated in a controlled way by using only one parameter: the temperature.
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Jan 2017
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