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At least 469 records · Page 26
All sourcesNASA NTRSDOE OSTI
DOE OSTI2014

Incorporation of La in epitaxial SrTiO{sub 3} thin films grown by atomic layer deposition on SrTiO{sub 3}-buffered Si (001) substrates

Strontium titanate, SrTiO{sub 3} (STO), thin films incorporated with lanthanum are grown on Si (001) substrates at a thickness range of 5–25 nm. Atomic layer deposition (ALD) is used to grow the La{sub x}Sr{sub 1−x}TiO{sub 3} (La:STO) films after buffering the Si (001) substrate with four-unit-cells of STO deposited by molecular beam epitaxy. The crystalline structure and orientation of the La:STO films are confirmed via reflection high-energy electron diffraction, X-ray diffraction, and cross-sectional transmission electron microscopy. The low temperature ALD growth (∼225 °C) and post-deposition annealing at 550 °C for 5 min maintains an abrupt interface between Si (001) and the crystalline oxide. Higher annealing temperatures (650 °C) show more complete La activation with film resistivities of ∼2.0 × 10{sup −2} Ω cm for 20-nm-thick La:STO (x ∼ 0.15); however, the STO-Si interface is slightly degraded due to the increased annealing temperature. To demonstrate the selective incorporation of lanthanum by ALD, a layered heterostructure is grown with an undoped STO layer sandwiched between two conductive La:STO layers. Based on this work, an epitaxial oxide stack centered on La:STO and BaTiO{sub 3} integrated with Si is envisioned as a material candidate for a ferroelectric field-effect transistor.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗
DOE OSTI2014

Low temperature thin film transistors with hollow cathode plasma-assisted atomic layer deposition based GaN channels

We report GaN thin film transistors (TFT) with a thermal budget below 250 °C. GaN thin films are grown at 200 °C by hollow cathode plasma-assisted atomic layer deposition (HCPA-ALD). HCPA-ALD-based GaN thin films are found to have a polycrystalline wurtzite structure with an average crystallite size of 9.3 nm. TFTs with bottom gate configuration are fabricated with HCPA-ALD grown GaN channel layers. Fabricated TFTs exhibit n-type field effect characteristics. N-channel GaN TFTs demonstrated on-to-off ratios (I{sub ON}/I{sub OFF}) of 10{sup 3} and sub-threshold swing of 3.3 V/decade. The entire TFT device fabrication process temperature is below 250 °C, which is the lowest process temperature reported for GaN based transistors, so far.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗
DOE OSTI2014

Characterization of CZTSSe photovoltaic device with an atomic layer-deposited passivation layer

We describe a CZTSSe (Cu{sub 2}ZnSn(S{sub 1−x},Se{sub x}){sub 4}) photovoltaic (PV) device with an ALD (atomic layer deposition) coated buffer dielectric layer for CZTSSe surface passivation. An ALD buffer layer, such as TiO{sub 2}, can be applied in order to reduce the interface recombination and improve the device's open-circuit voltage. Detailed characterization data including current-voltage, admittance spectroscopy, and capacitance profiling are presented in order to compare the performance of PV devices with and without the ALD layer.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗
DOE OSTI2014

Fabrication of AlN/BN bishell hollow nanofibers by electrospinning and atomic layer deposition

Aluminum nitride (AlN)/boron nitride (BN) bishell hollow nanofibers (HNFs) have been fabricated by successive atomic layer deposition (ALD) of AlN and sequential chemical vapor deposition (CVD) of BN on electrospun polymeric nanofibrous template. A four-step fabrication process was utilized: (i) fabrication of polymeric (nylon 6,6) nanofibers via electrospinning, (ii) hollow cathode plasma-assisted ALD of AlN at 100 °C onto electrospun polymeric nanofibers, (iii) calcination at 500 °C for 2 h in order to remove the polymeric template, and (iv) sequential CVD growth of BN at 450 °C. AlN/BN HNFs have been characterized for their chemical composition, surface morphology, crystal structure, and internal nanostructure using X-ray photoelectron spectroscopy, scanning electron microscopy, transmission electron microscopy, energy dispersive X-ray spectroscopy, and selected area electron diffraction. Measurements confirmed the presence of crystalline hexagonal BN and AlN within the three dimensional (3D) network of bishell HNFs with relatively low impurity content. In contrast to the smooth surface of the inner AlN layer, outer BN coating showed a highly rough 3D morphology in the form of BN nano-needle crystallites. It is shown that the combination of electrospinning and plasma-assisted low-temperature ALD/CVD can produce highly controlled multi-layered bishell nitride ceramic hollow nanostructures. While electrospinning enables easy fabrication of nanofibrous template, self-limiting reactions of plasma-assisted ALD and sequential CVD provide control over the wall thicknesses of AlN and BN layers with sub-nanometer accuracy.

36 MATERIALS SCIENCE↗
DOE OSTI2014

Integration of atomic layer deposited high-k dielectrics on GaSb via hydrogen plasma exposure

In this letter we report the efficacy of a hydrogen plasma pretreatment for integrating atomic layer deposited (ALD) high-k dielectric stacks with device-quality p-type GaSb(001) epitaxial layers. Molecular beam eptiaxy-grown GaSb surfaces were subjected to a 30 minute H{sub 2}/Ar plasma treatment and subsequently removed to air. High-k HfO{sub 2} and Al{sub 2}O{sub 3}/HfO{sub 2} bilayer insulating films were then deposited via ALD and samples were processed into standard metal-oxide-semiconductor (MOS) capacitors. The quality of the semiconductor/dielectric interface was probed by current-voltage and variable-frequency admittance measurements. Measurement results indicate that the H{sub 2}-plamsa pretreatment leads to a low density of interface states nearly independent of the deposited dielectric material, suggesting that pre-deposition H{sub 2}-plasma exposure, coupled with ALD of high-k dielectrics, may provide an effective means for achieving high-quality GaSb MOS structures for advanced Sb-based digital and analog electronics.

36 MATERIALS SCIENCE↗
DOE OSTI2015

Improved high temperature integration of Al{sub 2}O{sub 3} on MoS{sub 2} by using a metal oxide buffer layer

We deposited a metal oxide buffer layer before atomic layer deposition (ALD) of Al{sub 2}O{sub 3} onto exfoliated molybdenum disulfide (MoS{sub 2}) in order to accomplish enhanced integration. We demonstrate that even at a high temperature, functionalization of MoS{sub 2} by means of a metal oxide buffer layer can effectively provide nucleation sites for ALD precursors, enabling much better surface coverage of Al{sub 2}O{sub 3}. It is shown that using a metal oxide buffer layer not only allows high temperature ALD process, resulting in highly improved quality of Al{sub 2}O{sub 3}/MoS{sub 2} interface, but also leaves MoS{sub 2} intact.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗
DOE OSTI2015

Resistive switching and synaptic properties of fully atomic layer deposition grown TiN/HfO{sub 2}/TiN devices

Recently proposed novel neural network hardware designs imply the use of memristors as electronic synapses in 3D cross-bar architecture. Atomic layer deposition (ALD) is the most feasible technique to fabricate such arrays. In this work, we present the results of the detailed investigation of the gradual resistive switching (memristive) effect in nanometer thick fully ALD grown TiN/HfO{sub 2}/TiN stacks. The modelling of the I-V curves confirms interface limited trap-assisted-tunneling mechanism along the oxygen vacancies in HfO{sub 2} in all conduction states. The resistivity of the stack is found to critically depend upon the distance from the interface to the first trap in HfO{sub 2}. The memristive properties of ALD grown TiN/HfO{sub 2}/TiN devices are correlated with the demonstrated neuromorphic functionalities, such as long-term potentiation/depression and spike-timing dependent plasticity, thus indicating their potential as electronic synapses in neuromorphic hardware.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗
DOE OSTI2015

Work function tuning of plasma-enhanced atomic layer deposited WC{sub x}N{sub y} electrodes for metal/oxide/semiconductor devices

One of the main challenges facing the integration of metals as gate electrodes in advanced MOS devices is control over the Fermi level position at the metal/dielectric interface. In this study, we demonstrate the ability to tune the effective work function (EWF) of W-based electrodes by process modifications of the atomic layer deposited (ALD) films. Tungsten carbo-nitrides (WC{sub x}N{sub y}) films were deposited via plasma-enhanced and/or thermal ALD processes using organometallic precursors. The process modifications enabled us to control the stoichiometry of the WC{sub x}N{sub y} films. Deposition in hydrogen plasma (without nitrogen based reactant) resulted in a stoichiometry of WC{sub 0.4} with primarily W-C chemical bonding, as determined by x-ray photoelectron spectroscopy. These films yielded a relatively low EWF of 4.2 ± 0.1 eV. The introduction of nitrogen based reactant to the plasma or the thermal ALD deposition resulted in a stoichiometry of WC{sub 0.1}N{sub 0.6–0.8} with predominantly W-N chemical bonding. These films produced a high EWF of 4.7 ± 0.1 eV.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗
DOE OSTI2015

Comparison of gate dielectric plasma damage from plasma-enhanced atomic layer deposited and magnetron sputtered TiN metal gates

Fully depleted silicon-on-insulator transistors were fabricated using two different metal gate deposition mechanisms to compare plasma damage effects on gate oxide quality. Devices fabricated with both plasma-enhanced atomic-layer-deposited (PE-ALD) TiN gates and magnetron plasma sputtered TiN gates showed very good electrostatics and short-channel characteristics. However, the gate oxide quality was markedly better for PE-ALD TiN. A significant reduction in interface state density was inferred from capacitance-voltage measurements as well as a 1200× reduction in gate leakage current. A high-power magnetron plasma source produces a much higher energetic ion and vacuum ultra-violet (VUV) photon flux to the wafer compared to a low-power inductively coupled PE-ALD source. The ion and VUV photons produce defect states in the bulk of the gate oxide as well as at the oxide-silicon interface, causing higher leakage and potential reliability degradation.

36 MATERIALS SCIENCE↗
DOE OSTI2015

Electronic structure investigation of atomic layer deposition ruthenium(oxide) thin films using photoemission spectroscopy

Analyzing and manipulating the electronic band line-up of interfaces in novel micro- and nanoelectronic devices is important to achieve further advancement in this field. Such band alignment modifications can be achieved by introducing thin conformal interfacial dipole layers. Atomic layer deposition (ALD), enabling angstrom-precise control over thin film thickness, is an ideal technique for this challenge. Ruthenium (Ru{sup 0}) and its oxide (RuO{sub 2}) have gained interest in the past decade as interfacial dipole layers because of their favorable properties like metal-equivalent work functions, conductivity, etc. In this study, initial results of the electronic structure investigation of ALD Ru{sup 0} and RuO{sub 2} films via photoemission spectroscopy are presented. These experiments give insight into the band alignment, growth behavior, surface structure termination, and dipole formation. The experiments were performed in an integrated vacuum system attached to a home-built, stop-flow type ALD reactor without exposing the samples to the ambient in between deposition and analysis. Bis(ethylcyclopentadienyl)ruthenium(II) was used as precursor and oxygen as reactant. The analysis chamber was outfitted with X-ray photoemission spectroscopy (LIXPS, XPS). The determined growth modes are consistent with a strong growth inhibition situation with a maximum average growth rate of 0.21 Å/cycle for RuO{sub 2} and 0.04 Å/cycle for Ru.{sup 0} An interface dipole of up to −0.93 eV was observed, supporting the assumption of a strongly physisorbed interface. A separate experiment where the surface of a RuO film was sputtered suggests that the surface is terminated by an intermediate, stable, non-stoichiometric RuO{sub 2}/OH compound whose surface is saturated with hydroxyl groups.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗
DOE OSTI2015

Electrical properties of GaAs metal–oxide–semiconductor structure comprising Al{sub 2}O{sub 3} gate oxide and AlN passivation layer fabricated in situ using a metal–organic vapor deposition/atomic layer deposition hybrid system

This paper presents a compressive study on the fabrication and optimization of GaAs metal–oxide–semiconductor (MOS) structures comprising a Al{sub 2}O{sub 3} gate oxide, deposited via atomic layer deposition (ALD), with an AlN interfacial passivation layer prepared in situ via metal–organic chemical vapor deposition (MOCVD). The established protocol afforded self-limiting growth of Al{sub 2}O{sub 3} in the atmospheric MOCVD reactor. Consequently, this enabled successive growth of MOCVD-formed AlN and ALD-formed Al{sub 2}O{sub 3} layers on the GaAs substrate. The effects of AlN thickness, post-deposition anneal (PDA) conditions, and crystal orientation of the GaAs substrate on the electrical properties of the resulting MOS capacitors were investigated. Thin AlN passivation layers afforded incorporation of optimum amounts of nitrogen, leading to good capacitance–voltage (C–V) characteristics with reduced frequency dispersion. In contrast, excessively thick AlN passivation layers degraded the interface, thereby increasing the interfacial density of states (D{sub it}) near the midgap and reducing the conduction band offset. To further improve the interface with the thin AlN passivation layers, the PDA conditions were optimized. Using wet nitrogen at 600 °C was effective to reduce D{sub it} to below 2 × 10{sup 12} cm{sup −2} eV{sup −1}. Using a (111)A substrate was also effective in reducing the frequency dispersion of accumulation capacitance, thus suggesting the suppression of traps in GaAs located near the dielectric/GaAs interface. The current findings suggest that using an atmosphere ALD process with in situ AlN passivation using the current MOCVD system could be an efficient solution to improving GaAs MOS interfaces.

36 MATERIALS SCIENCE↗
DOE OSTI2015

Comparison of hydrolytic and non-hydrolytic atomic layer deposition chemistries: Interfacial electronic properties at alumina-silicon interfaces

We report the differences in the passivation and electronic properties of aluminum oxide (Al{sub 2}O{sub 3}) deposited on silicon via traditional hydrolytic atomic layer deposition (ALD) and non-hydrolytic (NH) ALD chemistries. Traditional films were grown using trimethylaluminum (TMA) and water and NHALD films grown using TMA and isopropanol at 300 °C. Hydrolytically grown ALD films contain a smaller amount of fixed charge than NHALD films (oxide fixed charge Q{sub f} {sub Traditional} = −8.1 × 10{sup 11 }cm{sup −2} and Q{sub f} {sub NHALD} = −3.6 × 10{sup 12 }cm{sup −2}), and a larger degree of chemical passivation than NHALD films (density of interface trap states, D{sub it} {sub Traditional} = 5.4 × 10{sup 11 }eV{sup −1 }cm{sup −2} and D{sub it} {sub NHALD} = 2.9 × 10{sup 12 }eV{sup −1 }cm{sup −2}). Oxides grown with both chemistries were found to have a band gap of 7.1 eV. The conduction band offset was 3.21 eV for traditionally grown films and 3.38 eV for NHALD. The increased D{sub it} for NHALD films may stem from carbon impurities in the oxide layer that are at and near the silicon surface, as evidenced by both the larger trap state time constant (τ{sub Traditional} = 2.2 × 10{sup −9} s and τ{sub NHALD} = 1.7 × 10{sup −7} s) and the larger carbon concentration. We have shown that the use of alcohol-based oxygen sources in NHALD chemistry can significantly affect the resulting interfacial electronic behavior presenting an additional parameter for understanding and controlling interfacial electronic properties at semiconductor-dielectric interfaces.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗
DOE OSTI2016

Low-temperature self-limiting atomic layer deposition of wurtzite InN on Si(100)

In this work, we report on self-limiting growth of InN thin films at substrate temperatures as low as 200 °C by hollow-cathode plasma-assisted atomic layer deposition (HCPA-ALD). The precursors used in growth experiments were trimethylindium (TMI) and N{sub 2} plasma. Process parameters including TMI pulse time, N{sub 2} plasma exposure time, purge time, and deposition temperature have been optimized for self-limiting growth of InN with in ALD window. With the increase in exposure time of N{sub 2} plasma from 40 s to 100 s at 200 °C, growth rate showed a significant decrease from 1.60 to 0.64 Å/cycle. At 200 °C, growth rate saturated as 0.64 Å/cycle for TMI dose starting from 0.07 s. Structural, optical, and morphological characterization of InN were carried out in detail. X-ray diffraction measurements revealed the hexagonal wurtzite crystalline structure of the grown InN films. Refractive index of the InN film deposited at 200 °C was found to be 2.66 at 650 nm. 48 nm-thick InN films exhibited relatively smooth surfaces with Rms surface roughness values of 0.98 nm, while the film density was extracted as 6.30 g/cm{sup 3}. X-ray photoelectron spectroscopy (XPS) measurements depicted the peaks of indium, nitrogen, carbon, and oxygen on the film surface and quantitative information revealed that films are nearly stoichiometric with rather low impurity content. In3d and N1s high-resolution scans confirmed the presence of InN with peaks located at 443.5 and 396.8 eV, respectively. Transmission electron microscopy (TEM) and selected area electron diffraction (SAED) further confirmed the polycrystalline structure of InN thin films and elemental mapping revealed uniform distribution of indium and nitrogen along the scanned area of the InN film. Spectral absorption measurements exhibited an optical band edge around 1.9 eV. Our findings demonstrate that HCPA-ALD might be a promising technique to grow crystalline wurtzite InN thin films at low substrate temperatures.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗
DOE OSTI2016

Effect of the nature of the substrate on the surface chemistry of atomic layer deposition precursors

The thermal chemistry of Cu(I)-sec-butyl-2-iminopyrrolidinate, a promising copper amidinate complex for atomic layer deposition (ALD) applications, was explored comparatively on several surfaces by using a combination of surface-sensitive techniques, specifically temperature-programmed desorption and x-ray photoelectron spectroscopy (XPS). The substrates explored include single crystals of transition metals (Ni(110) and Cu(110)), thin oxide films (NiO/Ni(110) and SiO 2 /Ta), and oxygen-treated metals (O/Cu(110)). Decomposition of the pyrrolidinate ligand leads to the desorption of several gas-phase products, including CH 3 CN, HCN and butene from the metals and CO and CO 2 from the oxygen-containing surfaces. In all cases dehydrogenation of the organic moieties is accompanied by hydrogen removal from the surface, in the form of H 2 on metals and mainly as water from the metal oxides, but the threshold for this chemistry varies wildly, from 270 K on Ni(110) to 430 K on O/Cu(110), 470 K on Cu(110), 500 K on NiO/Ni(110), and 570 K on SiO 2 /Ta. Here, copper reduction is also observed in both the Cu 2p 3/2 XPS and the Cu L 3 VV Auger (AES) spectra, reaching completion by 300 K on Ni(110) but occurring only between 500 and 600 K on Cu(110). On NiO/Ni(110), both Cu(I) and Cu(0) coexist between 200 and 500 K, and on SiO 2 /Ta a change happens between 500 and 600 K but the reduction is limited, with the copper atoms retaining a significant ionic character. Additional experiments to test adsorption at higher temperatures led to the identification of temperature windows for the self-limiting precursor uptake required for ALD between approximately 300 and 450 K on both Ni(110) and NiO/Ni(110); the range on SiO 2 had been previously determined to be wider, reaching an upper limit at about 500 K. Finally, deposition of copper metal films via ALD cycles with O 2 as the co-reactant was successfully accomplished on the Ni(110) substrate.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2018

Enhanced thermoelectric efficiency in topological insulator Bi 2 Te 3 nanoplates via atomic layer deposition-based surface passivation

We report in-plane thermoelectric measurements of Bi 2 Te 3 nanoplates, a typical topological insulator with Dirac-like metallic surface states, grown by chemical vapor deposition. The as-grown flakes exposed to ambient conditions exhibit relatively small thermopowers around -34 μV/K due to unintentional surface doping (e.g., gas adsorption and surface oxidation). After removal of the unintentional surface doping and surface passivation by deposition of 30 nm of Al 2 O 3 using atomic layer deposition (ALD), the Seebeck coefficient of these flakes increases by a factor of 5× to -169 μV/K. We believe that the ALD-based surface passivation can prevent the degradation of the thermoelectric properties caused by gas adsorption and surface oxidation processes, thus, reducing the unintentional doping in the Bi 2 Te 3 and increasing the Seebeck coefficient. The high surface-to-volume ratio of these thin (~10 nm thick) nanoplates make them especially sensitive to surface doping, which is a common problem among nanomaterials in general. An increase in the sample resistance is also observed after the ALD process, which is consistent with the decrease in doping.

36 MATERIALS SCIENCE↗
DOE OSTI2024

An automatic multi-precursor flow-type atomic layer deposition system

Designs for two automated atomic layer deposition (ALD) flow reactors are presented, and their capabilities for coating additively manufactured (AM) metal prints are described. One instrument allows the coating of several AM parts in batches, while the other is useful for single part experiments. To demonstrate reactor capabilities, alumina (Al 2 O 3 ) was deposited onto AM 316L stainless steel by dosing with water (H 2 O) vapor and trimethylaluminum (TMA) and purging with nitrogen gas (N 2 ). Both instruments are controlled by custom-programmed LabVIEW software that enables in situ logging of temperature, total pressure, and film thickness using a quartz crystal microbalance. An initial result shows that 150 ALD cycles led to a film thickness of ~55 nm, which was verified with Rutherford backscattering spectroscopy. This indicates that the reactors were indeed depositing single atomic layers of Al 2 O 3 per ALD cycle, as intended.

47 OTHER INSTRUMENTATION↗
DOE OSTI2025

Quantitative characterization of ZrO2 gate dielectric interface with tellurium

Tellurium (Te) has recently emerged as a promising p-type semiconductor that can be processed at low temperatures, compatible with back end of line CMOS integration. Characterization of tellurium–dielectric interfaces is essential for further device advancements. Here, the interface quality of Te with ZrO2 gate dielectric is studied in a metal-oxide semiconductor capacitor structure. The interface trap density (Dit) is measured as a function of atomic layer deposition (ALD) temperature, without the use of a seed layer. Given the low thermal budget of Te, the ALD temperature is shown to be particularly important. The lowest Dit of 5 × 1012 states/cm2 eV is obtained at a low ALD process temperature of 120 °C. To further assess the impact of Dit on device performance, field-effect transistors (FETs) were fabricated. The subthreshold swing and effective hole mobility of the FETs were analyzed in relation to Dit, emphasizing the importance of a defect-minimized interface for enhancing Te transistor performance.

Byeon, Kyeong-Jae↗
DOE OSTI2015

Pd nanoparticles on ZnO-passivated porous carbon by atomic layer deposition: an effective electrochemical catalyst for Li-O 2 battery

Uniformly dispersed Pd nanoparticles on ZnO-passivated porous carbon were synthesized via an atomic layer deposition (ALD) technique, which was tested as a cathode material in a rechargeable Li-O-2 battery, showing a highly active catalytic effect toward the electrochemical reactions-in particular, the oxygen evolution reaction. Transmission electron microscopy (TEM) showed discrete crystalline nanoparticles decorating the surface of the ZnO-passivated porous carbon support in which the size could be controlled in the range of 3-6 nm, depending on the number of Pd ALD cycles performed. X-ray absorption spectroscopy (XAS) at the Pd Kedge revealed that the carbon-supported Pd existed in a mixed phase of metallic palladium and palladium oxide. The ZnO-passivated layer effectively blocks the defect sites on the carbon surface, minimizing the electrolyte decomposition. Our results suggest that ALD is a promising technique for tailoring the surface composition and structure of nanoporous supports for Li-O-2 batteries.

77 NANOSCIENCE AND NANOTECHNOLOGY↗