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At least 883 records · Page 49

Synthesis of Pt 3 Zn 1 and Pt 1 Zn 1 intermetallic nanocatalysts for dehydrogenation of ethane

Pt 3 Zn 1 and Pt 1 Zn 1 intermetallic nanoparticles supported on SiO 2 were synthesized by combining atomic layer deposition (ALD) of ZnO, incipient wetness impregnation (IWI) of Pt, and appropriate hydrogen reduction. Here, the formation of Pt 1 Zn 1 and Pt 3 Zn 1 intermetallic nanoparticles was observed by both X-ray diffraction (XRD) and synchrotron X-ray absorption spectroscopy (XAS). STEM images showed that the 2–3 nm Pt-based intermetallic nanoparticles were uniformly dispersed on a SiO 2 support. The relationships between Pt–Zn intermetallic phases and synthesis conditions were established. In situ XAS measurements at Pt L 3 and Zn K edges during hydrogen reduction provided a detailed image of surface species evolution. Owing to a combined electronic and geometric effect, Pt 1 Zn 1 exhibited much higher reactivity and stability than Pt 3 Zn 1 and Pt in both the direct dehydrogenation and oxidative dehydrogenation of ethane to ethylene reactions.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Experimentally informed structure optimization of amorphous TiO 2 films grown by atomic layer deposition

Amorphous titanium dioxide TiO 2 (a-TiO 2 ) has been widely studied, particularly as a protective coating layer on semiconductors to prevent corrosion and promote electron–hole conduction in photoelectrochemical reactions. The stability and longevity of a-TiO 2 is strongly affected by the thickness and structural heterogeneity, implying that understanding the structure properties of a-TiO 2 is crucial for improving the performance. This study characterized the structural and electronic properties of a-TiO 2 thin films (~17 nm) grown on Si by atomic layer deposition (ALD). Fluctuation spectra V(k) and angular correlation functions were determined with 4-dimensional scanning transmission electron microscopy (4D-STEM), which revealed the distinctive medium-range ordering in the a-TiO 2 film. A realistic atomic model of a-TiO 2 was established guided by the medium-range ordering and the previously reported short-range ordering of a-TiO 2 film, as well as the interatomic potential. The structure was optimized by the StructOpt code using a genetic algorithm that simultaneously minimizes energy and maximizes the match to experimental short- and medium-range ordering. The StructOpt a-TiO 2 model presents improved agreements with the medium-range ordering and the k-space location of the dominant 2-fold angular correlations compared with a traditional melt-quenched model. The electronic structure of the StructOpt a-TiO 2 model was studied by ab initio calculations and compared to the crystalline phases and experimental results. Finally, this work uncovered the medium-range ordering in a-TiO 2 thin films and provided a realistic a-TiO 2 structure model for further investigation of structure–property relationships and materials design. In addition, the improved multi-objective optimization package StructOpt was provided for structure determination of complex materials guided by experiments and simulations.

36 MATERIALS SCIENCE↗

Interfacial band configuration and electrical properties of LaAlO{sub 3}/Al{sub 2}O{sub 3}/hydrogenated-diamond metal-oxide-semiconductor field effect transistors

In order to search a gate dielectric with high permittivity on hydrogenated-diamond (H-diamond), LaAlO{sub 3} films with thin Al{sub 2}O{sub 3} buffer layers are fabricated on the H-diamond epilayers by sputtering-deposition (SD) and atomic layer deposition (ALD) techniques, respectively. Interfacial band configuration and electrical properties of the SD-LaAlO{sub 3}/ALD-Al{sub 2}O{sub 3}/H-diamond metal-oxide-semiconductor field effect transistors (MOSFETs) with gate lengths of 10, 20, and 30 μm have been investigated. The valence and conduction band offsets of the SD-LaAlO{sub 3}/ALD-Al{sub 2}O{sub 3} structure are measured by X-ray photoelectron spectroscopy to be 1.1 ± 0.2 and 1.6 ± 0.2 eV, respectively. The valence band discontinuity between H-diamond and LaAlO{sub 3} is evaluated to be 4.0 ± 0.2 eV, showing that the MOS structure acts as the gate which controls a hole carrier density. The leakage current density of the SD-LaAlO{sub 3}/ALD-Al{sub 2}O{sub 3}/H-diamond MOS diode is smaller than 10{sup −8} A cm{sup −2} at gate bias from −4 to 2 V. The capacitance-voltage curve in the depletion mode shows sharp dependence, small flat band voltage, and small hysteresis shift, which implies low positive and trapped charge densities. The MOSFETs show p-type channel and complete normally off characteristics with threshold voltages changing from −3.6 ± 0.1 to −5.0 ± 0.1 V dependent on the gate length. The drain current maximum and the extrinsic transconductance of the MOSFET with gate length of 10 μm are −7.5 mA mm{sup −1} and 2.3 ± 0.1 mS mm{sup −1}, respectively. The enhancement mode SD-LaAlO{sub 3}/ALD-Al{sub 2}O{sub 3}/H-diamond MOSFET is concluded to be suitable for the applications of high power and high frequency electrical devices.

36 MATERIALS SCIENCE↗

Biexciton emission from single isoelectronic traps formed by nitrogen-nitrogen pairs in GaAs

We have studied photoluminescence (PL) from individual isoelectronic traps formed by nitrogen-nitrogen (NN) pairs in GaAs. Sharp emission lines due to exciton and biexciton were observed from individual isoelectronic traps in nitrogen atomic-layer doped (ALD) GaAs. The binding energy of biexciton bound to individual isoelectronic traps was approximately 8 meV. Both the exciton and biexciton luminescence lines show completely random polarization and no fine-structure splitting. These results are desirable to the application to the quantum cryptography used in the field of quantum information technology.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗

Plasmonic materials based on ZnO films and their potential for developing broadband middle-infrared absorbers

Noble metals such as gold and silver have been extensively used for plasmonic applications due to their ability to support plasmons, yet they suffer from high intrinsic losses. Alternative plasmonic materials that offer low loss and tunability are desired for a new generation of efficient and agile devices. In this paper, atomic layer deposition (ALD) grown ZnO is investigated as a candidate material for plasmonic applications. Optical constants of ZnO are investigated along with figures of merit pertaining to plasmonic waveguides. We show that ZnO can alleviate the trade-off between propagation length and mode confinement width owing to tunable dielectric properties. In order to demonstrate plasmonic resonances, we simulate a grating structure and computationally demonstrate an ultra-wide-band (4–15 μm) infrared absorber.

36 MATERIALS SCIENCE↗

Air-stable short-wave infrared PbS colloidal quantum dot photoconductors passivated with Al{sub 2}O{sub 3} atomic layer deposition

A PbS colloidal quantum dot photoconductor with Al{sub 2}O{sub 3} atomic layer deposition (ALD) passivation for air-stable operation is presented. Two different types of inorganic ligands for the quantum dots, S{sup 2−} and OH{sup −}, are investigated. PbS/S{sup 2−} photoconductors with a cut-off wavelength up to 2.4 μm are obtained, and a responsivity up to 50 A/W at 1550 nm is reported. The corresponding specific detectivity is ∼3.4 × 10{sup 8} Jones at 230 K. The 3-dB bandwidth of the PbS/S{sup 2−} and PbS/OH{sup −} photodetectors is 40 Hz and 11 Hz, respectively.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗

Effective reduction of trap density at the Y{sub 2}O{sub 3}/Ge interface by rigorous high-temperature oxygen annealing

The impact of thermal post deposition annealing in oxygen at different temperatures on the Ge/Y{sub 2}O{sub 3} interface is investigated using metal oxide semiconductor capacitors, where the yttrium oxide was grown by atomic layer deposition from tris(methylcyclopentadienyl)yttrium and H{sub 2}O precursors on n-type (100)-Ge substrates. By performing in-situ X-ray photoelectron spectroscopy, the growth of GeO during the first cycles of ALD was proven and interface trap densities just below 1 × 10{sup 11} eV{sup −1 }cm{sup −2} were achieved by oxygen annealing at high temperatures (550 °C–600 °C). The good interface quality is most likely driven by the growth of interfacial GeO{sub 2} and thermally stabilizing yttrium germanate.

36 MATERIALS SCIENCE↗

Vacuum ultraviolet photochemical selective area atomic layer deposition of Al{sub 2}O{sub 3} dielectrics

We report the photochemical atomic layer deposition of Al{sub 2}O{sub 3} thin films and the use of this process to achieve area-selective film deposition. A shuttered vacuum ultraviolet (VUV) light source is used to excite molecular oxygen and trimethyl aluminum to deposit films at 60°C. In-situ QCM and post-deposition ellipsometric measurements both show that the deposition rate is saturative as a function of irradiation time. Selective area deposition was achieved by projecting the VUV light through a metalized magnesium fluoride photolithographic mask and the selectivity of deposition on the illuminated and masked regions of the substrate is a logarithmic function of the UV exposure time. The Al{sub 2}O{sub 3} films exhibit dielectric constants of 8 – 10 at 1 MHz after forming gas annealing, similar to films deposited by conventional thermal ALD.

36 MATERIALS SCIENCE↗

Optimization of synthesis protocols to control the nanostructure and the morphology of metal oxide thin films for memristive applications

We propose a multi-technique approach based on in-vacuum synthesis of metal oxides to optimize the memristive properties of devices that use a metal oxide thin film as insulating layer. Pulsed Microplasma Cluster Source (PMCS) is based on supersonic beams seeded by clusters of the metal oxide. Nanocrystalline TiO{sub 2} thin films can be grown at room temperature, controlling the oxide stoichiometry from titanium metal up to a significant oxygen excess. Pulsed Electron beam Deposition (PED) is suitable to grow crystalline thin films on large areas, a step towards producing device arrays with controlled morphology and stoichiometry. Atomic Layer Deposition (ALD) is a powerful technique to grow materials layer-by-layer, finely controlling the chemical and structural properties of the film up to thickness of 50-80 nm. We will present a few examples of metal-insulator-metal structures showing a pinched hysteresis loop in their current-voltage characteristic. The structure, stoichiometry and morphology of the metal oxide layer, either aluminum oxide or titanium dioxide, is investigated by means of scanning electron microscopy (SEM) and by Raman scattering.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗

Hydroquinone-ZnO nano-laminate deposited by molecular-atomic layer deposition

In this study, we have deposited organic-inorganic hybrid semiconducting hydroquinone (HQ)/zinc oxide (ZnO) superlattices using molecular-atomic layer deposition, which enables accurate control of film thickness, excellent uniformity, and sharp interfaces at a low deposition temperature (150 °C). Self-limiting growth of organic layers is observed for the HQ precursor on ZnO surface. Nano-laminates were prepared by varying the number of HQ to ZnO cycles in order to investigate the physical and electrical effects of different HQ to ZnO ratios. It is indicated that the addition of HQ layer results in enhanced mobility and reduced carrier concentration. The highest Hall mobility of approximately 2.3 cm{sup 2}/V·s and the lowest n-type carrier concentration of approximately 1.0 × 10{sup 18}/cm{sup 3} were achieved with the organic-inorganic superlattice deposited with a ratio of 10 ZnO cycles to 1 HQ cycle. This study offers an approach to tune the electrical transport characteristics of ALD ZnO matrix thin films using an organic dopant. Moreover, with organic embedment, this nano-laminate material may be useful for flexible electronics.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗

Ferroelectricity in undoped hafnium oxide

We report the observation of ferroelectric characteristics in undoped hafnium oxide thin films in a thickness range of 4–20 nm. The undoped films were fabricated using atomic layer deposition (ALD) and embedded into titanium nitride based metal-insulator-metal (MIM) capacitors for electrical evaluation. Structural as well as electrical evidence for the appearance of a ferroelectric phase in pure hafnium oxide was collected with respect to film thickness and thermal budget applied during titanium nitride electrode formation. Using grazing incidence X-Ray diffraction (GIXRD) analysis, we observed an enhanced suppression of the monoclinic phase fraction in favor of an orthorhombic, potentially, ferroelectric phase with decreasing thickness/grain size and for a titanium nitride electrode formation below crystallization temperature. The electrical presence of ferroelectricity was confirmed using polarization measurements. A remanent polarization P{sub r} of up to 10 μC cm{sup −2} as well as a read/write endurance of 1.6 × 10{sup 5} cycles was measured for the pure oxide. The experimental results reported here strongly support the intrinsic nature of the ferroelectric phase in hafnium oxide and expand its applicability beyond the doped systems.

36 MATERIALS SCIENCE↗

Memristive behavior in a junctionless flash memory cell

We report charge storage based memristive operation of a junctionless thin film flash memory cell when it is operated as a two terminal device by grounding the gate. Unlike memristors based on nanoionics, the presented device mode, which we refer to as the flashristor mode, potentially allows greater control over the memristive properties, allowing rational design. The mode is demonstrated using a depletion type n-channel ZnO transistor grown by atomic layer deposition (ALD), with HfO{sub 2} as the tunnel dielectric, Al{sub 2}O{sub 3} as the control dielectric, and non-stoichiometric silicon nitride as the charge storage layer. The device exhibits the pinched hysteresis of a memristor and in the unoptimized device, R{sub off}/R{sub on} ratios of about 3 are presented with low operating voltages below 5 V. A simplified model predicts R{sub off}/R{sub on} ratios can be improved significantly by adjusting the native threshold voltage of the devices. The repeatability of the resistive switching is excellent and devices exhibit 10{sup 6 }s retention time, which can, in principle, be improved by engineering the gate stack and storage layer properties. The flashristor mode can find use in analog information processing applications, such as neuromorphic computing, where well-behaving and highly repeatable memristive properties are desirable.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗

In situ plasma enhanced atomic layer deposition half cycle study of Al{sub 2}O{sub 3} on AlGaN/GaN high electron mobility transistors

A half cycle study of plasma enhanced atomic layer deposited (PEALD) Al{sub 2}O{sub 3} on AlGaN is investigated using in situ X-ray photoelectron spectroscopy, low energy ion scattering, and ex situ electrical characterizations. A faster nucleation or growth is detected from PEALD relative to purely thermal ALD using an H{sub 2}O precursor. The remote O{sub 2} plasma oxidizes the AlGaN surface slightly at the initial stage, which passivates the surface and reduces the OFF-state leakage. This work demonstrates that PEALD is a useful strategy for Al{sub 2}O{sub 3} growth on AlGaN/GaN devices.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗

Correlation of interface states/border traps and threshold voltage shift on AlGaN/GaN metal-insulator-semiconductor high-electron-mobility transistors

In this paper, three electrical techniques (frequency dependent conductance analysis, AC transconductance (AC-g{sub m}), and positive gate bias stress) were used to evaluate three different gate dielectrics (Plasma-Enhanced Atomic Layer Deposition Si{sub 3}N{sub 4}, Rapid Thermal Chemical Vapor Deposition Si{sub 3}N{sub 4}, and Atomic Layer Deposition (ALD) Al{sub 2}O{sub 3}) for AlGaN/GaN Metal-Insulator-Semiconductor High-Electron-Mobility Transistors. From these measurements, the interface state density (D{sub it}), the amount of border traps, and the threshold voltage (V{sub TH}) shift during a positive gate bias stress can be obtained. The results show that the V{sub TH} shift during a positive gate bias stress is highly correlated to not only interface states but also border traps in the dielectric. A physical model is proposed describing that electrons can be trapped by both interface states and border traps. Therefore, in order to minimize the V{sub TH} shift during a positive gate bias stress, the gate dielectric needs to have a lower interface state density and less border traps. However, the results also show that the commonly used frequency dependent conductance analysis technique to extract D{sub it} needs to be cautiously used since the resulting value might be influenced by the border traps and, vice versa, i.e., the g{sub m} dispersion commonly attributed to border traps might be influenced by interface states.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗