Seungwu Han

Atomic structure of conducting nanofilaments in TiO2 resistive switching memory

Resistance switching in metal oxides could form the basis for next-generation non-volatile memory. It has been argued that the current in the high-conductivity state of several technologically relevant oxide materials flows through localized filaments, but these filaments have been characterized only indirectly, limiting our understanding of the switching mechanism. Here, we use high-resolution transmission electron microscopy to probe directly the nanofilaments in a Pt/TiO(2)/Pt system during resistive switching. In situ current-voltage and low-temperature (approximately 130 K) conductivity measurements confirm that switching occurs by the formation and disruption of Ti(n)O(2n-1) (or so-called Magnéli phase) filaments. Knowledge of the composition, structure and dimensions of these filaments will provide a foundation for unravelling the full mechanism of resistance switching in oxide thin films, and help guide research into the stability and scalability of such films for applications.

Development of new interatomic potentials appropriate for crystalline and liquid iron

Two procedures were developed to fit interatomic potentials of the embedded-atom method (EAM) form and applied to determine a potential which describes crystalline and liquid iron. While both procedures use perfect crystal and crystal defect data, the first procedure also employs the first-principles forces in a model liquid and the second procedure uses experimental liquid structure factor data. These additional types of information were incorporated to ensure more reasonable descriptions of atomic interactions at small separations than is provided using standard approaches, such as fitting to the universal binding energy relation. The new potentials (provided herein) are, on average, in better agreement with the experimental or first-principles lattice parameter, elastic constants, point-defect energies, bcc–fcc transformation energy, liquid density, liquid structure factor, melting temperature and other properties than other existing EAM iron potentials.

Electrical manipulation of nanofilaments in transition-metal oxides for resistance-based memory.

The fabrication of controlled nanostructures such as quantum dots, nanotubes, nanowires, and nanopillars has progressed rapidly over the past 10 years. However, both bottom-up and top-down methods to integrate the nanostructures are met with several challenges. For practical applications with the high level of the integration, an approach that can fabricate the required structures locally is desirable. In addition, the electrical signal to construct and control the nanostructures can provide significant advantages toward the stability and ordering. Through experiments on the negative resistance switching phenomenon in Pt-NiO-Pt structures, we have fabricated nanofilament channels that can be electrically connected or disconnected. Various analyses indicate that the nanofilaments are made of nickel and are formed at the grain boundaries. The scaling behaviors of the nickel nanofilaments were closely examined, with respect to the switching time, power, and resistance. In particular, the 100 nm x 100 nm cell was switchable on the nanosecond scale, making them ideal for the basis for high-speed, high-density, nonvolatile memory applications.

Development of an interatomic potential for phosphorus impurities in α-iron

We present the derivation of an interatomic potential for the iron–phosphorus system based primarily on ab initio data. Transferability in this system is extremely problematic, and the potential is intended specifically to address the problem of radiation damage and point defects in iron containing low concentrations of phosphorus atoms. Some preliminary molecular dynamics calculations show that P strongly affects point defect migration.We present the derivation of an interatomic potential for the iron phosphorus system based primarily on {\it ab initio} data. Transferrability in this system is extremely problematic, and the potential is intended specifically to address the problem of radiation damage and point defects in iron containing low concentrations of phosphorus atoms. Some preliminary molecular dynamics calculations show that P strongly affects point defect migration.

Hydrated Manganese(II) Phosphate (Mn3(PO4)2·3H2O) as a Water Oxidation Catalyst

The development of a water oxidation catalyst has been a demanding challenge in realizing water splitting systems. The asymmetric geometry and flexible ligation of the biological Mn4CaO5 cluster are important properties for the function of photosystem II, and these properties can be applied to the design of new inorganic water oxidation catalysts. We identified a new crystal structure, Mn3(PO4)2·3H2O, that precipitates spontaneously in aqueous solution at room temperature and demonstrated its high catalytic performance under neutral conditions. The bulky phosphate polyhedron induces a less-ordered Mn geometry in Mn3(PO4)2·3H2O. Computational analysis indicated that the structural flexibility in Mn3(PO4)2·3H2O could stabilize the Jahn-Teller-distorted Mn(III) and thus facilitate Mn(II) oxidation. This study provides valuable insights into the interplay between atomic structure and catalytic activity.

A detailed understanding of the electronic bipolar resistance switching behavior in Pt/TiO2/Pt structure

The detailed mechanism of electronic bipolar resistance switching (BRS) in the Pt/TiO(2)/Pt structure was examined. The conduction mechanism analysis showed that the trap-free and trap-mediated space-charge-limited conduction (SCLC) governs the low and high resistance state of BRS, respectively. The SCLC was confirmed by fitting the current-voltage characteristics of low and high resistance states at various temperatures. The BRS behavior originated from the asymmetric potential barrier for electrons escaping from, and trapping into, the trap sites with respect to the bias polarity. This asymmetric potential barrier was formed at the interface between the trap layer and trap-free layer. The detailed parameters such as trap density, and trap layer and trap-free layer thicknesses in the electronic BRS were evaluated. This showed that the degradation in the switching performance could be understood from the decrease and modified distribution of the trap densities in the trap layer.

First-principles modeling of resistance switching in perovskite oxide material

We report a first-principles study on SrRuO3∕SrTiO3 interface in the presence of the oxygen vacancy. While the oxygen vacancy on the side of SrTiO3 significantly lowers the Schottky barrier height, the oxygen vacancy close to the interface or inside the metallic electrode results in a Schottky barrier comparable to that of the clean interface. Based on these results, we propose a model for resistance-switching phenomena in perovskite oxide∕metal interfaces where electromigration of the oxygen vacancy plays a key role. Our model provides a consistent explanation of a recent experiment on resistance switching in SrRuO3∕Nb:SrTiO3 interface.

Anion control as a strategy to achieve high-mobility and high-stability oxide thin-film transistors

Ultra-definition, large-area displays with three-dimensional visual effects represent megatrend in the current/future display industry. On the hardware level, such a “dream” display requires faster pixel switching and higher driving current, which in turn necessitate thin-film transistors (TFTs) with high mobility. Amorphous oxide semiconductors (AOS) such as In-Ga-Zn-O are poised to enable such TFTs, but the trade-off between device performance and stability under illumination critically limits their usability, which is related to the hampered electron-hole recombination caused by the oxygen vacancies. Here we have improved the illumination stability by substituting oxygen with nitrogen in ZnO, which may deactivate oxygen vacancies by raising valence bands above the defect levels. Indeed, the stability under illumination and electrical bias is superior to that of previous AOS-based TFTs. By achieving both mobility and stability, it is highly expected that the present ZnON TFTs will be extensively deployed in next-generation flat-panel displays.

N-doped monolayer graphene catalyst on silicon photocathode for hydrogen production

Carbon-based catalysts have been attracting attention in renewable energy technologies due to the low cost and high stability, but their insufficient activity is still a challenging issue. Here, we suggest that monolayer graphene can be used as a catalyst for solar-driven hydrogen evolution reaction on Si-photocathodes, and its catalytic activity is boosted by plasma treatment in N2-ambient. The plasma treatment induces abundant defects and the incorporation of nitrogen atoms in the graphene structure, which can act as catalytic sites on graphene. The monolayer graphene containing nitrogen impurities exhibits a remarkable increase in the exchange current density and leads to a significant anodic shift of the onset of photocurrent from the Si-photocathode. Additionally, monolayer graphene shows the passivation effect that suppresses the surface oxidation of Si, thus enabling the operation of the Si-photocathode in neutral water. This study shows that graphene itself can be applied to a photoelectrochemical system as a catalyst with high activity and chemical stability.

Role of structural defects in the unipolar resistive switching characteristics of Pt∕NiO∕Pt structures

We investigated the resistive switching characteristics of two types of Pt∕NiO∕Pt structures with epitaxial and polycrystalline NiO layers. Both of these Pt∕NiO∕Pt structures exhibited unipolar resistive switching. Pt/epitaxial-NiO∕Pt showed unstable switching or no resistance state change after several repeated runs. Pt/polycrystalline-NiO∕Pt showed very reproducible switching. The experimental data indicated that microstructural defects (e.g., grain boundaries) played crucial roles in the reliability of the unipolar resistive switching behavior. This was further supported by first-principles calculations.