Sangmoon Yoon

Concave Rhombic Dodecahedral Au Nanocatalyst with Multiple High-Index Facets for CO2 Reduction

A concave rhombic dodecahedron (RD) gold nanoparticle was synthesized by adding 4-aminothiophenol (4-ATP) during growth from seeds. This shape is enclosed by stabilized facets of various high-indexes, such as (331), (221), and (553). Because it is driven thermodynamically and stabilized by 4-ATP ligands, the concave RD maintains its structure over a few months, even after rigorous electrochemical reactions. We discussed the mechanism of the shape evolution controlled by 4-ATP and found that both the binding energy of Au-S and the aromatic geometry of 4-ATP are major determinants of Au atom deposition during growth. As a possible application, we demonstrated that the concave RD exhibits superior electrocatalytic performance for the selective conversion of CO2 to CO in aqueous solution.

Ordered growth of topological insulator Bi2Se3 thin films on dielectric amorphous SiO2 by MBE

Topological insulators (TIs) are exotic materials which have topologically protected states on the surface due to strong spin-orbit coupling. However, a lack of ordered growth of TI thin films on amorphous dielectrics and/or insulators presents a challenge for applications of TI-junctions. We report the growth of topological insulator Bi2Se3 thin films on amorphous SiO2 by molecular beam epitaxy (MBE). To achieve the ordered growth of Bi2Se3 on an amorphous surface, the formation of other phases at the interface is suppressed by Se passivation. Structural characterizations reveal that Bi2Se3 films are grown along the [001] direction with a good periodicity by the van der Waals epitaxy mechanism. A weak anti-localization effect of Bi2Se3 films grown on amorphous SiO2 shows a modulated electrical property by the gating response. Our approach for ordered growth of Bi2Se3 on an amorphous dielectric surface presents considerable advantages for TI-junctions with amorphous insulator or dielectric thin films.

High‐Resolution Observation of Nucleation and Growth Behavior of Nanomaterials Using a Graphene Template

By using graphene as an electron beam-transparent substrate for both nanomaterial growth and transmission electron microscopy (TEM) measurements, we investigate initial growth behavior of nanomaterials. The direct growth and imaging method using graphene facilitate atomic-resolution imaging of nanomaterials at the very early stage of growth. This enables the observation of the transition in crystal structure of ZnO nuclei and the formation of various defects during nanomaterial growth.

Latent Order in High-Angle Grain Boundary of GaN

We report the existence of latent order during core relaxation in the high-angle grain boundaries (GBs) of GaN films using atomic-resolution scanning transmission electron microscopy and ab initio density functional theory calculations. Core structures in the high-angle GBs are characterized by two pairs of Ga-N bonds located next to each other. The core type correlates strongly with the bond angle differences. We identify an order of core relaxation hidden in the high-angle GBs by further classifying the 5/7 atom cores into a stable 5/7 core (5/7(S)) and a metastable 5/7 core (5/7(M)). This core-type classification indicates that metastable cores can exist at real high-angle GBs under certain circumstances. Interestingly, 5/7(M) exhibits distinct defect states compared to 5/7(S), despite their similar atomic configurations. We investigate the reconstruction of defect states observed in 5/7(M) by analyzing the real-space wave functions. An inversion occurred between two localized states during the transition from 5/7(S) to 5/7(M). We suggest an inversion mechanism to explain the formation of new defect states in 5/7(M).

Understanding luminescence properties of grain boundaries in GaN thin films and their atomistic origin

We report our findings on the optical properties of grain boundaries in GaN films grown on graphene layers and discuss their atomistic origin. We combine electron backscatter diffraction with cathodoluminescence to directly correlate the structural defects with their optical properties, enabling the high-precision local luminescence measurement of the grain boundaries in GaN films. To further understand the atomistic origin of the luminescence properties, we carefully probed atomic core structures of the grain boundaries by exploiting aberration-corrected scanning transmission electron microscopy. The atomic core structures of grain boundaries show different ordering behaviors compared with those observed previously in threading dislocations. Energetics of the grain boundary core structures and their correlation with electronic structures were studied by first principles calculation.