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Description

Novel hydride chemistries are employed to deposit light-emitting Ge1-y Snyalloys with y ≤ 0.1 by Ultra-High Vacuum Chemical Vapor Deposition (UHV-CVD) on Ge-buffered Si wafers. The properties of the resultant materials are systematically compared with similar alloys grown directly on Si wafers. The fundamental difference between the two systems is a fivefold

Novel hydride chemistries are employed to deposit light-emitting Ge1-y Snyalloys with y ≤ 0.1 by Ultra-High Vacuum Chemical Vapor Deposition (UHV-CVD) on Ge-buffered Si wafers. The properties of the resultant materials are systematically compared with similar alloys grown directly on Si wafers. The fundamental difference between the two systems is a fivefold (and higher) decrease in lattice mismatch between film and virtual substrate, allowing direct integration of bulk-like crystals with planar surfaces and relatively low dislocation densities. For y ≤ 0.06, the CVD precursors used were digermane Ge2H6 and deuterated stannane SnD4. For y ≥ 0.06, the Ge precursor was changed to trigermane Ge3H8, whose higher reactivity enabled the fabrication of supersaturated samples with the target film parameters. In all cases, the Ge wafers were produced using tetragermane Ge4H10 as the Ge source. The photoluminescence intensity from Ge1-y Sny /Ge films is expected to increase relative to Ge1-y Sny /Si due to the less defected interface with the virtual substrate. However, while Ge1-y Sny /Si films are largely relaxed, a significant amount of compressive strain may be present in the Ge1-y Sny /Ge case. This compressive strain can reduce the emission intensity by increasing the separation between the direct and indirect edges. In this context, it is shown here that the proposed CVD approach to Ge1-y Sny /Ge makes it possible to approach film thicknesses of about 1  μm, for which the strain is mostly relaxed and the photoluminescence intensity increases by one order of magnitude relative to Ge1-y Sny /Si films. The observed strain relaxation is shown to be consistent with predictions from strain-relaxation models first developed for the Si1-x Gex /Si system. The defect structure and atomic distributions in the films are studied in detail using advanced electron-microscopy techniques, including aberration corrected STEM imaging and EELS mapping of the average diamond–cubic lattice.

ContributorsSenaratne, Charutha Lasitha (Author) / Gallagher, J. D. (Author) / Jiang, Liying (Author) / Aoki, Toshihiro (Author) / Smith, David (Author) / Menéndez, Jose (Author) / Kouvetakis, John (Author) / Department of Chemistry and Biochemistry (Contributor)
Created2014-10-07
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Description

In this paper, we report on the highly conductive layer formed at the crystalline γ-alumina/SrTiO3 interface, which is attributed to oxygen vacancies. We describe the structure of thin γ-alumina layers deposited by molecular beam epitaxy on SrTiO3 (001) at growth temperatures in the range of 400–800 °C, as determined by reflection-high-energy

In this paper, we report on the highly conductive layer formed at the crystalline γ-alumina/SrTiO3 interface, which is attributed to oxygen vacancies. We describe the structure of thin γ-alumina layers deposited by molecular beam epitaxy on SrTiO3 (001) at growth temperatures in the range of 400–800 °C, as determined by reflection-high-energy electron diffraction, x-ray diffraction, and high-resolution electron microscopy. In situ x-ray photoelectron spectroscopy was used to confirm the presence of the oxygen-deficient layer. Electrical characterization indicates sheet carrier densities of ∼1013 cm−2 at room temperature for the sample deposited at 700 °C, with a maximum electron Hall mobility of 3100 cm2V-1s-1 at 3.2 K and room temperature mobility of 22 cm2V-1s-1. Annealing in oxygen is found to reduce the carrier density and turn a conductive sample into an insulator.

ContributorsKormondy, Kristy J. (Author) / Posadas, Agham B. (Author) / Ngo, Thong Q. (Author) / Lu, Sirong (Author) / Goble, Nicholas (Author) / Jordan-Sweet, Jean (Author) / Gao, Xuan P. A. (Author) / Smith, David (Author) / McCartney, Martha (Author) / Ekerdt, John G. (Author) / Demkov, Alexander A. (Author) / College of Liberal Arts and Sciences (Contributor)
Created2015-03-07
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Description

The development of non-volatile logic through direct coupling of spontaneous ferroelectric polarization with semiconductor charge carriers is nontrivial, with many issues, including epitaxial ferroelectric growth, demonstration of ferroelectric switching and measurable semiconductor modulation. Here we report a true ferroelectric field effect—carrier density modulation in an underlying Ge(001) substrate by switching

The development of non-volatile logic through direct coupling of spontaneous ferroelectric polarization with semiconductor charge carriers is nontrivial, with many issues, including epitaxial ferroelectric growth, demonstration of ferroelectric switching and measurable semiconductor modulation. Here we report a true ferroelectric field effect—carrier density modulation in an underlying Ge(001) substrate by switching of the ferroelectric polarization in epitaxial c-axis-oriented BaTiO3 grown by molecular beam epitaxy. Using the density functional theory, we demonstrate that switching of BaTiO3 polarization results in a large electric potential change in Ge. Aberration-corrected electron microscopy confirms BaTiO3 tetragonality and the absence of any low-permittivity interlayer at the interface with Ge. The non-volatile, switchable nature of the single-domain out-of-plane ferroelectric polarization of BaTiO3 is confirmed using piezoelectric force microscopy. The effect of the polarization switching on the conductivity of the underlying Ge is measured using microwave impedance microscopy, clearly demonstrating a ferroelectric field effect.

ContributorsPonath, Patrick (Author) / Fredrickson, Kurt (Author) / Posadas, Agham B. (Author) / Ren, Yuan (Author) / Wu, Xiaoyu (Author) / Vasudevan, Rama K. (Author) / Okatan, M. Baris (Author) / Jesse, S. (Author) / Aoki, Toshihiro (Author) / McCartney, Martha (Author) / Smith, David (Author) / Kalinin, Sergei V. (Author) / Lai, Keji (Author) / Demkov, Alexander A. (Author) / Ira A. Fulton Schools of Engineering (Contributor)
Created2015-01-01
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Description

We report a study of the magnetic domain structure of nanocrystalline thin films of nickel-zinc ferrite. The ferrite films were synthesized using aqueous spin-spray coating at low temperature (∼90 °C) and showed high complex permeability in the GHz range. Electron microscopy and microanalysis revealed that the films consisted of columnar grains

We report a study of the magnetic domain structure of nanocrystalline thin films of nickel-zinc ferrite. The ferrite films were synthesized using aqueous spin-spray coating at low temperature (∼90 °C) and showed high complex permeability in the GHz range. Electron microscopy and microanalysis revealed that the films consisted of columnar grains with uniform chemical composition. Off-axis electron holography combined with magnetic force microscopy indicated a multi-grain domain structure with in-plane magnetization. The correlation between the magnetic domain morphology and crystal structure is briefly discussed.

ContributorsZhang, D. (Author) / Ray, N. M. (Author) / Petuskey, William (Author) / Smith, David (Author) / McCartney, Martha (Author) / Ira A. Fulton Schools of Engineering (Contributor)
Created2014-08-28
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Description

The current work explores the crystalline perovskite oxide, strontium hafnate, as a potential high-k gate dielectric for Ge-based transistors. SrHfO3 (SHO) is grown directly on Ge by atomic layer deposition and becomes crystalline with epitaxial registry after post-deposition vacuum annealing at ∼700 °C for 5 min. The 2 × 1 reconstructed, clean Ge (001)

The current work explores the crystalline perovskite oxide, strontium hafnate, as a potential high-k gate dielectric for Ge-based transistors. SrHfO3 (SHO) is grown directly on Ge by atomic layer deposition and becomes crystalline with epitaxial registry after post-deposition vacuum annealing at ∼700 °C for 5 min. The 2 × 1 reconstructed, clean Ge (001) surface is a necessary template to achieve crystalline films upon annealing. The SHO films exhibit excellent crystallinity, as shown by x-ray diffraction and transmission electron microscopy. The SHO films have favorable electronic properties for consideration as a high-k gate dielectric on Ge, with satisfactory band offsets (>2 eV), low leakage current (<10-5 A/cm2 at an applied field of 1 MV/cm) at an equivalent oxide thickness of 1 nm, and a reasonable dielectric constant (k ∼ 18). The interface trap density (Dit) is estimated to be as low as ∼2 × 1012 cm-2 eV-1 under the current growth and anneal conditions. Some interfacial reaction is observed between SHO and Ge at temperatures above ∼650 °C, which may contribute to increased Dit value. This study confirms the potential for crystalline oxides grown directly on Ge by atomic layer deposition for advanced electronic applications.

ContributorsMcDaniel, Martin D. (Author) / Hu, Chengqing (Author) / Lu, Sirong (Author) / Ngo, Thong Q. (Author) / Posadas, Agham (Author) / Jiang, Aiting (Author) / Smith, David (Author) / Yu, Edward T. (Author) / Demkov, Alexander A. (Author) / Ekerdt, John G. (Author) / College of Liberal Arts and Sciences (Contributor)
Created2015-02-07
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Description

The sensitivity of Earth’s wetlands to observed shifts in global precipitation and temperature patterns and their ability to produce large quantities of methane gas are key global change questions. We present a microwave satellite-based approach for mapping fractional surface water (FW) globally at 25-km resolution. The approach employs a land

The sensitivity of Earth’s wetlands to observed shifts in global precipitation and temperature patterns and their ability to produce large quantities of methane gas are key global change questions. We present a microwave satellite-based approach for mapping fractional surface water (FW) globally at 25-km resolution. The approach employs a land cover-supported, atmospherically-corrected dynamic mixture model applied to 20+ years (1992–2013) of combined, daily, passive/active microwave remote sensing data. The resulting product, known as Surface Water Microwave Product Series (SWAMPS), shows strong microwave sensitivity to sub-grid scale open water and inundated wetlands comprising open plant canopies. SWAMPS’ FW compares favorably (R2 = 91%–94%) with higher-resolution, global-scale maps of open water from MODIS and SRTM-MOD44W. Correspondence of SWAMPS with open water and wetland products from satellite SAR in Alaska and the Amazon deteriorates when exposed wetlands or inundated forests captured by the SAR products were added to the open water fraction reflecting SWAMPS’ inability to detect water underneath the soil surface or beneath closed forest canopies. Except for a brief period of drying during the first 4 years of observation, the inundation extent for the global domain excluding the coast was largely stable. Regionally, inundation in North America is advancing while inundation is on the retreat in Tropical Africa and North Eurasia. SWAMPS provides a consistent and long-term global record of daily FW dynamics, with documented accuracies suitable for hydrologic assessment and global change-related investigations.

ContributorsSchroeder, Ronny (Author) / McDonald, Kyle C. (Author) / Chapman, Bruce D. (Author) / Jensen, Katherine (Author) / Podest, Erika (Author) / Tessler, Zachary D. (Author) / Bohn, Theodore (Author) / Zimmermann, Reiner (Author) / College of Liberal Arts and Sciences (Contributor)
Created2015-12-09
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Description

A warming climate is altering land-atmosphere exchanges of carbon, with a potential for increased vegetation productivity as well as the mobilization of permafrost soil carbon stores. Here we investigate land-atmosphere carbon dioxide (CO2) cycling through analysis of net ecosystem productivity (NEP) and its component fluxes of gross primary productivity (GPP)

A warming climate is altering land-atmosphere exchanges of carbon, with a potential for increased vegetation productivity as well as the mobilization of permafrost soil carbon stores. Here we investigate land-atmosphere carbon dioxide (CO2) cycling through analysis of net ecosystem productivity (NEP) and its component fluxes of gross primary productivity (GPP) and ecosystem respiration (ER) and soil carbon residence time, simulated by a set of land surface models (LSMs) over a region spanning the drainage basin of Northern Eurasia. The retrospective simulations cover the period 1960–2009 at 0.5° resolution, which is a scale common among many global carbon and climate model simulations. Model performance benchmarks were drawn from comparisons against both observed CO2 fluxes derived from site-based eddy covariance measurements as well as regional-scale GPP estimates based on satellite remote-sensing data.

The site-based comparisons depict a tendency for overestimates in GPP and ER for several of the models, particularly at the two sites to the south. For several models the spatial pattern in GPP explains less than half the variance in the MODIS MOD17 GPP product. Across the models NEP increases by as little as 0.01 to as much as 0.79 g C m-2 yr-2, equivalent to 3 to 340 % of the respective model means, over the analysis period. For the multimodel average the increase is 135 % of the mean from the first to last 10 years of record (1960–1969 vs. 2000–2009), with a weakening CO2 sink over the latter decades. Vegetation net primary productivity increased by 8 to 30 % from the first to last 10 years, contributing to soil carbon storage gains. The range in regional mean NEP among the group is twice the multimodel mean, indicative of the uncertainty in CO2 sink strength.

The models simulate that inputs to the soil carbon pool exceeded losses, resulting in a net soil carbon gain amid a decrease in residence time. Our analysis points to improvements in model elements controlling vegetation productivity and soil respiration as being needed for reducing uncertainty in land-atmosphere CO2 exchange. These advances will require collection of new field data on vegetation and soil dynamics, the development of benchmarking data sets from measurements and remote-sensing observations, and investments in future model development and intercomparison studies.

ContributorsRawlins, M. A. (Author) / McGuire, A. D. (Author) / Kimball, J. S. (Author) / Dass, P. (Author) / Lawrence, D. (Author) / Burke, E. (Author) / Chen, X. (Author) / Delire, C. (Author) / Koven, C. (Author) / MacDougall, A. (Author) / Peng, S. (Author) / Rinke, A. (Author) / Saito, K. (Author) / Zhang, W. (Author) / Alkama, R. (Author) / Bohn, Theodore (Author) / Ciais, P. (Author) / Decharme, B. (Author) / Gouttevin, I. (Author) / Hajima, T. (Author) / Ji, D. (Author) / Krinner, G. (Author) / Lettenmaier, D. P. (Author) / Miller, P. (Author) / Moore, J. C. (Author) / Smith, B. (Author) / Sueyoshi, T. (Author) / College of Liberal Arts and Sciences (Contributor)
Created2015-07-28
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Description

Soil temperature (Ts) change is a key indicator of the dynamics of permafrost. On seasonal and interannual timescales, the variability of Ts determines the active-layer depth, which regulates hydrological soil properties and biogeochemical processes. On the multi-decadal scale, increasing Ts not only drives permafrost thaw/retreat but can also trigger and

Soil temperature (Ts) change is a key indicator of the dynamics of permafrost. On seasonal and interannual timescales, the variability of Ts determines the active-layer depth, which regulates hydrological soil properties and biogeochemical processes. On the multi-decadal scale, increasing Ts not only drives permafrost thaw/retreat but can also trigger and accelerate the decomposition of soil organic carbon. The magnitude of permafrost carbon feedbacks is thus closely linked to the rate of change of soil thermal regimes. In this study, we used nine process-based ecosystem models with permafrost processes, all forced by different observation-based climate forcing during the period 1960–2000, to characterize the warming rate of Ts in permafrost regions. There is a large spread of Ts trends at 20 cm depth across the models, with trend values ranging from 0.010 ± 0.003 to 0.031 ± 0.005 °C yr-1. Most models show smaller increase in Ts with increasing depth. Air temperature (Tsub>a) and longwave downward radiation (LWDR) are the main drivers of Ts trends, but their relative contributions differ amongst the models. Different trends of LWDR used in the forcing of models can explain 61 % of their differences in Ts trends, while trends of Ta only explain 5 % of the differences in Ts trends. Uncertain climate forcing contributes a larger uncertainty in Ts trends (0.021 ± 0.008 °C yr-1, mean ± standard deviation) than the uncertainty of model structure (0.012 ± 0.001 °C yr-1), diagnosed from the range of response between different models, normalized to the same forcing. In addition, the loss rate of near-surface permafrost area, defined as total area where the maximum seasonal active-layer thickness (ALT) is less than 3 m loss rate, is found to be significantly correlated with the magnitude of the trends of Ts at 1 m depth across the models (R = −0.85, P = 0.003), but not with the initial total near-surface permafrost area (R = −0.30, P = 0.438). The sensitivity of the total boreal near-surface permafrost area to Ts at 1 m is estimated to be of −2.80 ± 0.67 million km2°C-1. Finally, by using two long-term LWDR data sets and relationships between trends of LWDR and Ts across models, we infer an observation-constrained total boreal near-surface permafrost area decrease comprising between 39 ± 14  ×  103 and 75 ± 14  ×  103km2yr-1 from 1960 to 2000. This corresponds to 9–18 % degradation of the current permafrost area.

ContributorsPeng, S. (Author) / Ciais, P. (Author) / Krinner, G. (Author) / Wang, T. (Author) / Gouttevin, I. (Author) / McGuire, A. D. (Author) / Lawrence, D. (Author) / Burke, E. (Author) / Chen, X. (Author) / Decharme, B. (Author) / Koven, C. (Author) / MacDougall, A. (Author) / Rinke, A. (Author) / Saito, K. (Author) / Zhang, W. (Author) / Alkama, R. (Author) / Bohn, Theodore (Author) / Delire, C. (Author) / Hajima, T. (Author) / Ji, D. (Author) / Lettenmaier, D. P. (Author) / Miller, P. A. (Author) / Moore, J. C. (Author) / Smith, B. (Author) / Sueyoshi, T. (Author) / College of Liberal Arts and Sciences (Contributor)
Created2016-01-20
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Description

A realistic simulation of snow cover and its thermal properties are important for accurate modelling of permafrost. We analyse simulated relationships between air and near-surface (20  cm) soil temperatures in the Northern Hemisphere permafrost region during winter, with a particular focus on snow insulation effects in nine land surface models,

A realistic simulation of snow cover and its thermal properties are important for accurate modelling of permafrost. We analyse simulated relationships between air and near-surface (20  cm) soil temperatures in the Northern Hemisphere permafrost region during winter, with a particular focus on snow insulation effects in nine land surface models, and compare them with observations from 268 Russian stations. There are large cross-model differences in the simulated differences between near-surface soil and air temperatures (ΔT; 3 to 14 °C), in the sensitivity of soil-to-air temperature (0.13 to 0.96 °C °C-1), and in the relationship between ΔT and snow depth. The observed relationship between ΔT and snow depth can be used as a metric to evaluate the effects of each model's representation of snow insulation, hence guide improvements to the model's conceptual structure and process parameterisations. Models with better performance apply multilayer snow schemes and consider complex snow processes. Some models show poor performance in representing snow insulation due to underestimation of snow depth and/or overestimation of snow conductivity. Generally, models identified as most acceptable with respect to snow insulation simulate reasonable areas of near-surface permafrost (13.19 to 15.77 million  km2). However, there is not a simple relationship between the sophistication of the snow insulation in the acceptable models and the simulated area of Northern Hemisphere near-surface permafrost, because several other factors, such as soil depth used in the models, the treatment of soil organic matter content, hydrology and vegetation cover, also affect the simulated permafrost distribution.

ContributorsWang, Wenli (Author) / Rinke, Annette (Author) / Moore, John C. (Author) / Ji, Duoying (Author) / Cui, Xuefeng (Author) / Peng, Shushi (Author) / Lawrence, David M. (Author) / McGuire, A. David (Author) / Burke, Eleanor J. (Author) / Chen, Xiaodong (Author) / Decharme, Bertrand (Author) / Koven, Charles (Author) / MacDougall, Andrew (Author) / Saito, Kazuyuki (Author) / Zhang, Wenxin (Author) / Alkama, Ramdane (Author) / Bohn, Theodore (Author) / Ciais, Philippe (Author) / Delire, Christine (Author) / Gouttevin, Isabelle (Author) / Hajima, Tomohiro (Author) / Krinner, Gerhard (Author) / Lettenmaier, Dennis P. (Author) / Miller, Paul A. (Author) / Smith, Benjamin (Author) / Sueyoshi, Tetsuo (Author) / Sherstiukov, Artem B. (Author) / College of Liberal Arts and Sciences (Contributor)
Created2016-08-11
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Description

The (110) plane of Co3O4 spinel exhibits significantly higher rates of carbon monoxide conversion due to the presence of active Co3+ species at the surface. However, experimental studies of Co3O4 (110) surfaces and interfaces have been limited by the difficulties in growing high-quality films. We report thin (10–250 Å) Co3O4 films

The (110) plane of Co3O4 spinel exhibits significantly higher rates of carbon monoxide conversion due to the presence of active Co3+ species at the surface. However, experimental studies of Co3O4 (110) surfaces and interfaces have been limited by the difficulties in growing high-quality films. We report thin (10–250 Å) Co3O4 films grown by molecular beam epitaxy in the polar (110) direction on MgAl2O4 substrates. Reflection high-energy electron diffraction, atomic force microscopy, x-ray diffraction, and transmission electron microscopy measurements attest to the high quality of the as-grown films. Furthermore, we investigate the electronic structure of this material by core level and valence band x-ray photoelectron spectroscopy, and first-principles density functional theory calculations. Ellipsometry reveals a direct band gap of 0.75 eV and other interband transitions at higher energies. A valence band offset of 3.2 eV is measured for the Co3O4/MgAl2O4 heterostructure. Magnetic measurements show the signature of antiferromagnetic ordering at 49 K. FTIR ellipsometry finds three infrared-active phonons between 300 and 700 cm-1.

ContributorsKormondy, Kristy J. (Author) / Posadas, Agham B. (Author) / Slepko, Alexander (Author) / Dhamdhere, Ajit (Author) / Smith, David (Author) / Mitchell, Khadijih N. (Author) / Willett-Gies, Travis I. (Author) / Zollner, Stefan (Author) / Marshall, Luke G. (Author) / Zhou, Jianshi (Author) / Demkov, Alexander A. (Author) / College of Liberal Arts and Sciences (Contributor)
Created2014-06-28