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Register a new userDirect imaging of liquid-nanoparticle interface with atom probe tomography
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Understanding the structure and chemical composition at the liquid-nanoparticle (NP) interface is crucial for a wide range of physical, chemical and biological processes. In this study, direct imaging of the liquid-NP interface by atom probe tomography (APT) is reported for the first time, which reveals the distributions and the interactions of key atoms and molecules in this critical domain. The APT specimen is prepared by controlled graphene encapsulation of the solution containing nanoparticles on a metal tip, with an end radius in the range of 50 nm to allow field ionization and evaporation. Using Au nanoparticles (AuNPs) in suspension as an example, analysis of the mass spectrum and three-dimensional (3D) chemical maps from APT provides a detailed image of the water-gold interface with near-atomic resolution. At the water-gold interface, the formation of an electrical double layer (EDL) rich in water (H2O) molecules has been observed, which results from the charge from the binding between the trisodium-citrate layer and the AuNP. In the bulk water region, the density of reconstructed H2O has been shown to be consistent, reflecting a highly packed density of H2O molecules after graphene encapsulation. This study is the first demonstration of direct imaging of liquid-NP interface using APT with results providing an atom-by-atom 3D dissection of the liquid-NP interface.
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We report first principles theory based electronic structure studies of a semiconducting stoichiometric cage-like Cd9Te9 cluster. Substantial changes are observed in the electronic structure of the cluster on passivation with fictitious hydrogen atoms, in particular, widening of the energy gap between highest occupied molecular orbital and lowest unoccupied molecular orbital and enhancement in stability of cluster is seen. The cluster, when substitutionally mono-doped for a Cd by a set of 3d and 4d transition metal atoms (Ti, V, Cr, Mn, Fe, Co, Ni, Cu, Zn, Ru, Rh and Pd), is found to acquire polarization as seen from spin resolved density of states near Fermi level. Further, such mono-doping in passivated cluster shows half-metallic behavior. Mapping of partial density of states of each system on that of undoped cluster reveals additional levels caused by doping each TM atom separately. In the 3d elemental doping, Ti and Mn doping result into electron type doping whereas all other cases result into hole doped systems. For all the 4d elements studied, it is akin to the doping with holes for Cd substitution in the outer ring, whereas for Ru and Rh, there is electron type doping in case of substitution for Cd in central ring upon passivation. A comparison of partial density of states plots for bare and passivated clusters, on doping with transition metal atoms, suggests suitability of the cage-like cluster for spintronics applications.
Introducing magnetic order into a topological insulator (TI) system has been attracting much attention with an expectation of realizing exotic phenomena such as quantum anomalous Hall effect (QAHE) or axion insulator states. The magnetic proximity effect (MPE) is one of the promising schemes to induce the magnetic order on the surface of TI without introducing disorder accompanied by doping magnetic impurities in TI. In this study, we investigate the MPE at the interface of a heterostructure consisting of a topological crystalline insulator (TCI) SnTe and Fe by employing polarized neutron reflectometry. The ferromagnetic order penetrates $sim$ 3 nm deep into the SnTe layer from the interface with Fe, which persists up to room temperature. Our findings demonstrate that the interfacial magnetism is induced by the MPE on the surface of TCI preserving the coherent topological states, which is essential for the bulk-edge correspondence, without introducing disorder arising from a random distribution magnetic impurities. This opens up a way for realizing next generation electronics, spintronics, and quantum computational devices by making use of the characteristics of TCI.
The atomic structure at the interface between a two-dimensional (2D) and a three-dimensional (3D) material influences properties such as contact resistance, photo-response, and high-frequency performance. Moire engineering has yet to be explored for tailoring this 2D/3D interface, despite its success in enabling correlated physics at 2D/2D twisted van der Waals interfaces. Using epitaxially aligned MoS$_2$ /Au{111} as a model system, we apply a geometric convolution technique and four-dimensional scanning transmission electron microscopy (4D STEM) to show that the 3D nature of the Au structure generates two coexisting moire periods (18 Angstroms and 32 Angstroms) at the 2D/3D interface that are otherwise hidden in conventional electron microscopy imaging. We show, via ab initio electronic structure calculations, that charge density is modulated with the longer of these moire periods, illustrating the potential for (opto-)electronic modulation via moire engineering at the 2D/3D interface.
We use electronic transport and atom probe tomography to study ZnO:Al / SiO2 / Si Schottky junctions on lightly-doped n- and p-type Si. We vary the carrier concentration in the the ZnO:Al films by two orders of magnitude but the Schottky barrier height remains constant, consistent with Fermi level pinning seen in metal / Si junctions. Atom probe tomography shows that Al segregates to the interface, so that the ZnO:Al at the junction is likely to be metallic even when the bulk of the ZnO:Al film is semiconducting. We hypothesize that Fermi level pinning is connected to the insulator-metal transition in doped ZnO, and that controlling this transition may be key to un-pinning the Fermi level in oxide / Si Schottky junctions.
The process of homogeneous crystal nucleation has been considered in a model liquid, where the interparticle interaction is described by a short-range spherical oscillatory potential. Mechanisms of initiating structural ordering in the liquid at various supercooling levels, including those corresponding to an amorphous state, have been determined. The sizes and shapes of formed crystal grains have been estimated statistically. The results indicate that the mechanisms of nucleation occurs throughout the entire considered temperature range. The crystallization of the system at low supercooling levels occurs through a mononuclear scenario. A high concentration of crystal nuclei formed at high supercooling levels (i.e., at temperatures comparable to and below the glass transition temperature $T_g$) creates the semblance of the presence of branched structures, which is sometimes erroneously interpreted as a signature of phase separation. The temperature dependence of the maximum concentration of crystal grains demonstrates two regimes the transition between which occurs at a temperature comparable to the glass transition temperature $T_g$.
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