Z.S. Szilagyi

Bio: Z.S. Szilagyi is an academic researcher. The author has contributed to research in topics: Scanning transmission electron microscopy & Spherical aberration. The author has an hindex of 9, co-authored 26 publications receiving 2224 citations.

Atom-by-atom structural and chemical analysis by annular dark-field electron microscopy

Abstract: An imaging technique able to resolve and identify all individual atoms in non-periodic solids would be a very useful tool for materials analysis. Annular dark-field (ADF) imaging in an aberration-corrected scanning transmission electron microscope optimized for low voltage operation allows such an analysis, as shown by Ondrej Krivanek and co-workers. The technique was used to examine a monolayer of boron nitride, in which it revealed individual atomic substitutions involving carbon and oxygen impurity atoms. Careful analysis of the data enables the construction of a detailed map of the atomic structure, with all the atoms of the four species resolved and identified. An imaging technique that could identify all the individual atoms, including defects, in a material would be a useful tool. Here an electron-microscopy approach to the problem, based on annular dark-field imaging, is described. A monolayer of boron nitride was studied, and three types of atomic substitution were identified. Careful analysis of the data enabled the construction of a detailed map of the atomic structure. Direct imaging and chemical identification of all the atoms in a material with unknown three-dimensional structure would constitute a very powerful general analysis tool. Transmission electron microscopy should in principle be able to fulfil this role, as many scientists including Feynman realized early on1. It images matter with electrons that scatter strongly from individual atoms and whose wavelengths are about 50 times smaller than an atom. Recently the technique has advanced greatly owing to the introduction of aberration-corrected optics2,3,4,5,6,7,8. However, neither electron microscopy nor any other experimental technique has yet been able to resolve and identify all the atoms in a non-periodic material consisting of several atomic species. Here we show that annular dark-field imaging in an aberration-corrected scanning transmission electron microscope optimized for low voltage operation can resolve and identify the chemical type of every atom in monolayer hexagonal boron nitride that contains substitutional defects. Three types of atomic substitutions were found and identified: carbon substituting for boron, carbon substituting for nitrogen, and oxygen substituting for nitrogen. The substitutions caused in-plane distortions in the boron nitride monolayer of about 0.1 A magnitude, which were directly resolved, and verified by density functional theory calculations. The results demonstrate that atom-by-atom structural and chemical analysis of all radiation-damage-resistant atoms present in, and on top of, ultra-thin sheets has now become possible.

Direct Sub-Angstrom Imaging of a Crystal Lattice

Abstract: Despite the use of electrons with wavelengths of just a few picometers, spatial resolution in a transmission electron microscope (TEM) has been limited by spherical aberration to typically around 0.15 nanometer. Individual atomic columns in a crystalline lattice can therefore only be imaged for a few low-order orientations, limiting the range of defects that can be imaged at atomic resolution. The recent development of spherical aberration correctors for transmission electron microscopy allows this limit to be overcome. We present direct images from an aberration-corrected scanning TEM that resolve a lattice in which the atomic columns are separated by less than 0.1 nanometer.

High-energy-resolution monochromator for aberration-corrected scanning transmission electron microscopy/electron energy-loss spectroscopy

Abstract: An all-magnetic monochromator/spectrometer system for sub-30 meV energy-resolution electron energy-loss spectroscopy in the scanning transmission electron microscope is described. It will link the energy being selected by the monochromator to the energy being analysed by the spectrometer, without resorting to decelerating the electron beam. This will allow it to attain spectral energy stability comparable to systems using monochromators and spectrometers that are raised to near the high voltage of the instrument. It will also be able to correct the chromatic aberration of the probe-forming column. It should be able to provide variable energy resolution down to approximately 10 meV and spatial resolution less than 1 A.

Single-atom catalysis of CO oxidation using Pt1/FeOx

Abstract: Platinum-based heterogeneous catalysts are critical to many important commercial chemical processes, but their efficiency is extremely low on a per metal atom basis, because only the surface active-site atoms are used. Catalysts with single-atom dispersions are thus highly desirable to maximize atom efficiency, but making them is challenging. Here we report the synthesis of a single-atom catalyst that consists of only isolated single Pt atoms anchored to the surfaces of iron oxide nanocrystallites. This single-atom catalyst has extremely high atom efficiency and shows excellent stability and high activity for both CO oxidation and preferential oxidation of CO in H-2. Density functional theory calculations show that the high catalytic activity correlates with the partially vacant 5d orbitals of the positively charged, high-valent Pt atoms, which help to reduce both the CO adsorption energy and the activation barriers for CO oxidation.

Progress, Challenges, and Opportunities in Two-Dimensional Materials Beyond Graphene

Abstract: Graphene’s success has shown that it is possible to create stable, single and few-atom-thick layers of van der Waals materials, and also that these materials can exhibit fascinating and technologically useful properties. Here we review the state-of-the-art of 2D materials beyond graphene. Initially, we will outline the different chemical classes of 2D materials and discuss the various strategies to prepare single-layer, few-layer, and multilayer assembly materials in solution, on substrates, and on the wafer scale. Additionally, we present an experimental guide for identifying and characterizing single-layer-thick materials, as well as outlining emerging techniques that yield both local and global information. We describe the differences that occur in the electronic structure between the bulk and the single layer and discuss various methods of tuning their electronic properties by manipulating the surface. Finally, we highlight the properties and advantages of single-, few-, and many-layer 2D materials in...

Recent Advances in Ultrathin Two-Dimensional Nanomaterials

Abstract: Since the discovery of mechanically exfoliated graphene in 2004, research on ultrathin two-dimensional (2D) nanomaterials has grown exponentially in the fields of condensed matter physics, material science, chemistry, and nanotechnology. Highlighting their compelling physical, chemical, electronic, and optical properties, as well as their various potential applications, in this Review, we summarize the state-of-art progress on the ultrathin 2D nanomaterials with a particular emphasis on their recent advances. First, we introduce the unique advances on ultrathin 2D nanomaterials, followed by the description of their composition and crystal structures. The assortments of their synthetic methods are then summarized, including insights on their advantages and limitations, alongside some recommendations on suitable characterization techniques. We also discuss in detail the utilization of these ultrathin 2D nanomaterials for wide ranges of potential applications among the electronics/optoelectronics, electrocat...

One-dimensional electrical contact to a two-dimensional material.

Abstract: Heterostructures based on layering of two-dimensional (2D) materials such as graphene and hexagonal boron nitride represent a new class of electronic devices. Realizing this potential, however, depends critically on the ability to make high-quality electrical contact. Here, we report a contact geometry in which we metalize only the 1D edge of a 2D graphene layer. In addition to outperforming conventional surface contacts, the edge-contact geometry allows a complete separation of the layer assembly and contact metallization processes. In graphene heterostructures, this enables high electronic performance, including low-temperature ballistic transport over distances longer than 15 micrometers, and room-temperature mobility comparable to the theoretical phonon-scattering limit. The edge-contact geometry provides new design possibilities for multilayered structures of complimentary 2D materials.