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Search indexed NASA NTRS and DOE OSTI research on propulsion, heat transfer, battery materials and energy systems. Follow report and document links to the original sources.

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At least 505 records · Page 28
All sourcesNASA NTRSDOE OSTI
DOE OSTI2023

Kirigami Photopiezo Catalysts for Self-Sustainable Environment Remediation

Photo(electro)-piezo catalysis has emerged as one of the most effective strategies for sustainable environmental remediation. While various (nano)materials have been investigated for enhancing the intrinsic properties related to the interfacial band structure, increasing the efficiency by integration of materials with rational design for stress–strain applications has not yet been considered. Herein, we introduce kirigami strain engineering to photopiezo catalysts for enhancing efficiency by increasing the magnitude of applied strain and density of bends. Macroscale stretching motion is converted into localized bending by a pliable kirigami structure using similar or even lower input energy, which can be easily modulated by natural waves. The kirigami structure leads to a significant enhancement (~250%) in the degradation of dyes, and we discovered the significant contribution of the oxygen reduction pathway in the charge-transfer mechanism, which corresponds to the observed enhancement. In conclusion, the photopiezo catalytic effects of kirigami were further highlighted by the small water reservoir test, showing its feasibility in nature for self-sustainable environmental remediation that can be modulated using motions of winds, waves, and life vibrations.

14 SOLAR ENERGY↗
DOE OSTI2020

Mechanistic Insight into Lignin Slow Pyrolysis by Linking Pyrolysis Chemistry and Carbon Material Properties

As a highly abundant renewable carbon source, lignin can be converted to a variety of advanced carbon materials with tailorable properties through slow pyrolysis. In this study, slow pyrolysis of kraft lignin, for the first time, was investigated with a commercial pyrolysis–gas chromatography–mass spectrometry (Py–GC–MS) system through evolved gas analysis-MS (EGA-MS) and heart-cutting-GC–MS (HC-GC–MS) analyses. These analyses allow recovery and examination of the multiphased gas products generated from thermal decomposition of lignin during slow pyrolysis at a controlled heating rate over a long time course, thus making it possible to link operation conditions, pyrolysis chemistry, and carbon material properties. The overall product distributions, including volatiles and solid products, were quantitatively tracked at different heating rates (2, 20, and 40 °C/min) and different temperature regions (100–200, 200–300, and 300–600 °C). Solid residues were further characterized using a suite of analytical tools, in correlation with the investigation of formation mechanisms of volatiles to reveal the reaction chemistry of lignin during slow pyrolysis and to determine the morphology, pore structure, and interfacial chemical properties. This study provides critical insights into the slow pyrolysis chemistry of lignin and the properties of the resulting carbon material. These results will facilitate a better design and control of the lignin slow pyrolysis process for synthesizing functional carbon materials.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2024

Modeling Si/SiGe quantum dot variability induced by interface disorder reconstructed from multiperspective microscopy

SiGe heteroepitaxial growth yields pristine host material for quantum dot qubits, but residual interface disorder can lead to qubit-to-qubit variability that might pose an obstacle to reliable SiGe-based quantum computing. By convolving data from scanning tunneling microscopy and high-angle annular dark field scanning transmission electron microscopy, we reconstruct 3D interfacial atomic structure and employ an atomistic multi-valley effective mass theory to quantify qubit spectral variability. The results indicate (1) appreciable valley splitting (VS) variability of ~50% owing to alloy disorder and (2) roughness-induced double-dot detuning bias energy variability of order 1–10 meV depending on well thickness. For measured intermixing, atomic steps have negligible influence on VS, and uncorrelated roughness causes spatially fluctuating energy biases in double-dot detunings potentially incorrectly attributed to charge disorder. Our approach yields atomic structure spanning orders of magnitude larger areas than post-growth microscopy or tomography alone, enabling more holistic predictions of disorder-induced qubit variability.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗
DOE OSTI2016

Visualising the molecular alteration of the calcite (104) – water interface by sodium nitrate

The reactivity of calcite, one of the most abundant minerals in the earth’s crust, is determined by the molecular details of its interface with the contacting solution. Recently, it has been found that trace concentrations of NaNO 3 severely affect calcite’s (104) surface and its reactivity. Here we combine molecular dynamics (MD) simulations, X-ray reflectivity (XR) and in situ atomic force microscopy (AFM) to probe the calcite (104) – water interface in the presence of NaNO 3 . Simulations reveal density profiles of different ions near calcite’s surface, with NO 3 – able to reach closer to the surface than CO 3 2– and in higher concentrations. Reflectivity measurements show a structural destabilisation of the (104) surfaces’ topmost atomic layers in NaNO 3 bearing solution, with distorted rotation angles of the carbonate groups and substantial displacement of the lattice ions. Nanoscale AFM results confirm the alteration of crystallographic characteristics, and the ability of dissolved NaNO 3 to modify the structure of interfacial water was observed by AFM force spectroscopy. Our experiments and simulations consistently evidence a dramatic deterioration of the crystals’ surface, with potentially important implications for geological and industrial processes.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2020

A redox-active organic cation for safer high energy density Li-ion batteries

Ni-rich layered cathode materials are at the forefront to be deployed in high energy density Li-ion batteries for the automotive market. However, the intrinsic poor structural and interfacial stability during overcharging could trigger violent thermal failure, which severely limits their wide application. To protect the Ni-rich cathode from overcharging, we firstly report a redox-active cation, thioether-substituted diaminocyclopropenium, as an electrolyte additive to limit the cell voltage within the safe value during overcharging. The organic cation demonstrates a record-breaking electrochemical reversibility at ~4.55 V versus Li + /Li and solubility (0.5 M) in carbonate-based electrolyte. The protection capability of the additive was explored in two cell chemistries: a LiNi 0.8 Co 0.15 Al 0.05 O 2 /graphite cell and a LiNi 0.8 Co 0.15 Al 0.05 O 2 /silicon–graphene cell with areal capacities of ~2.2 mA h cm -2 and ~3 mA h cm -2 , respectively. With 0.2 M addition, the LiNi 0.8 Co 0.15 Al 0.05 O 2 /graphite cell survived 54 cycles at 0.2C with 100% overcharge. Moreover, the cell can carry an utmost 4.4 mA cm -2 (2C) with 100% overcharge and a maximum capacity of 7540% SOC at 0.2C.

25 ENERGY STORAGE↗
DOE OSTI2011

High-resolution core-level photoemission study of CF{sub 4}-treated Gd{sub 2}O{sub 3}(Ga{sub 2}O{sub 3}) gate dielectric on Ge probed by synchrotron radiation

High-resolution core-level photoemission analysis using synchrotron radiation was used to investigate the superior electrical performance of aGa{sub 2}O{sub 3}(Gd{sub 2}O{sub 3}) gate dielectric on Ge(001) after CF{sub 4} treatment. Prior to the treatment, a thin germanate-like oxide layer that formed at the interface prevented Ge from diffusing to the surface. The Ge surface retained a small amount of buckled dimers from the as-grown sample. The buckled dimers were quickly removed by CF{sub 4} plasma treatment followed by an annealing process, resulting in a more uniform interface than that of the as-grown sample. The detailed interfacial electronic structure for the untreated and treated samples are presented.

36 MATERIALS SCIENCE↗
DOE OSTI2011

Interfacial energy level bending in a crystalline p/p-type organic heterostructure

A conduction channel was observed at the heterointerface of the crystalline p-type organic films copper phthalocyanine (CuPc) and 2,5-bis(4-biphenylyl) bithiophene (BP2T). Energy level bending at the interface is confirmed by photoemission spectroscopy, which verifies a charge transfer between CuPc and BP2T. This provides a further route to utilize interfacial electronic properties in functional devices and also documents the importance of reconsidering the interfacial electronic structure of organic heterostructures.

36 MATERIALS SCIENCE↗
DOE OSTI2012

Hard x-ray photoelectron spectroscopy study on band alignment at poly(3,4-ethylenedioxythiophene):poly(styrenesulfonate)/ZnO interface

We used hard x-ray photoelectron spectroscopy to investigate the interfacial electronic states of a poly(styrenesulfonate) doped poly(3,4-ethylenedioxythiophene) (PEDOT:PSS) contact on a ZnO single crystal. An understanding of the interfacial band structure is useful for putting the organic contact to practical use. We observed upward band bending of the ZnO layer a few nanometers from the interface. The detected ZnO bulk region exhibited a flat band structure, meaning that the PEDOT:PSS does not greatly deplete the ZnO layer. The band bending caused the charge injection barrier formation with the result that the contact exhibited the Schottky property.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗
DOE OSTI2012

Energy level alignment at the interfaces between typical electrodes and nucleobases: Al/adenine/indium-tin-oxide and Al/thymine/indium-tin-oxide

We investigated the interfacial electronic structures of Al/adenine/indium-tin-oxide (ITO) and Al/thymine/ITO using in situ ultraviolet and x-ray photoemission spectroscopy and density functional theory calculations. Adenine shows both an interface dipole and level bending, whereas thymine shows only an interface dipole in contact with ITO. In addition, thymine possesses a larger ionization energy than adenine. These are understood with delocalized {pi} states confirmed with theoretical calculations. For the interface between nucleobases and Al, both nucleobases show a prominent reduction of the electron injection barrier from Al to each base in accordance with a downward level shift.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗
DOE OSTI2013

Magnetic manipulation by resistance switching in CeO{sub 2}/PrBa{sub 2}Cu{sub 3}O{sub 7−δ}/Pt heterostructure: The role of oxygen vacancies

Pronounced bipolar resistance switching with a good retention property has been observed in CeO{sub 2}/PrBa{sub 2}Cu{sub 3}O{sub 7−δ}/Pt heterostructure. The low resistance state and high resistance state exhibited distinguished ferromagnetic signals, as compared to the nearly non-magnetic initial state. It is found that the migration of the oxygen vacancies under electric field is mainly responsible for the electric and the magnetic changes. The modified interfacial electronic structure by the oxygen vacancy migration and the trapping/detrapping of the carriers leads to the resistance switching. The exchange interaction of the hydrogen-like orbitals formed around the singly occupied oxygen vacancies in CeO{sub 2} is accounting for the emerged and modulated ferromagnetic signals. Temperature dependence of resistance in the low resistance state follows a variable range hopping law, further confirming that the amount of oxygen vacancies in the CeO{sub 2} layer directly affects the hydrogen-like orbital radius, which determines the strength of the ferromagnetic coupling.

36 MATERIALS SCIENCE↗
DOE OSTI2014

Spin dependent transport properties of Mn-Ga/MgO/Mn-Ga magnetic tunnel junctions with metal(Mg, Co, Cr) insertion layer

We report a first principles theoretical investigation of spin polarized quantum transport in Mn{sub 2}Ga/MgO/Mn{sub 2}Ga and Mn{sub 3}Ga/MgO/Mn{sub 3}Ga magnetic tunneling junctions (MTJs) with the consideration of metal(Mg, Co, Cr) insertion layer effect. By changing the concentration of Mn, our calculation shows a considerable disparity in transport properties: A tunneling magnetoresistance (TMR) ratio of 852% was obtained for Mn{sub 2}Ga-based MTJs, however, only a 5% TMR ratio for Mn{sub 3}Ga-based MTJs. In addition, the influence of insertion layer has been considered in our calculation. We found the Co insertion layer can increase the TMR of Mn{sub 2}Ga-based MTJ to 904%; however, the Cr insertion layer can decrease the TMR by 668%; A negative TMR ratio can be obtained with Mg insertion layer. Our work gives a comprehensive understanding of the influence of different insertion layer in Mn-Ga based MTJs. It is proved that, due to the transmission can be modulated by the interfacial electronic structure of insertion, the magnetoresistance ratio of Mn{sub 2}Ga/MgO/Mn{sub 2}Ga MTJ can be improved by inserting Co layer.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗
DOE OSTI2014

Theory of third-order spectroscopic methods to extract detailed molecular orientational dynamics for planar surfaces and other uniaxial systems

Functionalized organic monolayers deposited on planar two-dimensional surfaces are important systems for studying ultrafast orientational motions and structures of interfacial molecules. Several studies have successfully observed the orientational relaxation of functionalized monolayers by fluorescence depolarization experiments and recently by polarization-resolved heterodyne detected vibrational transient grating (HDTG) experiments. In this article we provide a model-independent theory to extract orientational correlation functions unique to interfacial molecules and other uniaxial systems based on polarization-resolved resonant third-order spectroscopies, such as pump-probe spectroscopy, HDTG spectroscopy, and fluorescence depolarization experiment. It will be shown (in the small beam-crossing angle limit) that five measurements are necessary to completely characterize the monolayer's motions: I{sub ∥}(t) and I{sub ⊥}(t) with the incident beams normal to the surface, I{sub ∥}(t) and I{sub ⊥}(t) with a non-zero incident angle, and a time averaged linear dichroism measurement. Once these measurements are performed, two orientational correlation functions corresponding to in-plane and out-of-plane motions are obtained. The procedure is applicable not only for monolayers on flat surfaces, but any samples with uniaxial symmetry such as uniaxial liquid crystals and aligned planar bilayers. The theory is valid regardless of the nature of the actual molecular motions on interface. We then apply the general results to wobbling-in-a-cone model, in which molecular motions are restricted to a limited range of angles. Within the context of the model, the cone angle, the tilt of the cone relative to the surface normal, and the orientational diffusion constant can be determined. The results are extended to describe analysis of experiments where the beams are not crossing in the small angle limit.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2014

Effect of interfacial layer on the crystal structure of InAs/AlAs{sub 0.16}Sb{sub 0.84}/AlSb quantum wells

Ion channeling technique using MeV C{sup 2+} ions and high resolution X-ray diffraction were used to study the crystal quality of an InAs/AlSb-based quantum wells. We found that the InAs quality has a strong dependence on the type of the interface used. With the addition of the InSb-like interface, the crystal quality of the InAs channel was greatly improved. The InAs lattice was fully strained and aligned with the lattice of the buffer layer without any lattice relaxation. On the other hand, if the interface was of the AlAs type, the lattice of the InAs quantum well was relaxed and the crystal quality was poor. This explains why a superior InAs quantum well with high electron mobility and good surface morphology can be achieved with the use of the InSb interface.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗
DOE OSTI2014

Carrier behavior in special multilayer device composed of different transition metal oxide-based intermediate connectors

The impact of illumination on the connection part of the tandem organic light-emitting diodes was studied by using a special organic multilayer sample consisted of two organic active layers coupled with different transition metal oxide (TMO)-based intermediate connectors (ICs). Through measuring the current density-voltage characteristic, interfacial electronic structures, and capacitance-voltage characteristic, we observe an unsymmetrical phenomenon in current density-voltage and capacitance-voltage curves of Mg:Alq{sub 3}/MoO{sub 3} and MoO{sub 3} composed devices, which was induced by the charge spouting zone near the ICs region and the recombination state in the MoO{sub 3} layer. Moreover, Mg:Alq{sub 3}/MoO{sub 3} composed device displays a photovoltaic effect and the V{sub oc} shifts to forward bias under illumination. Our results demonstrate that the TMO-based IC structure coupled with photovoltaic effect can be a good approach for the study of photodetector, light sensor, and so on.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗
DOE OSTI2015

Interfacial Ga-As suboxide: Structural and electronic properties

The structural and electronic properties of Ga-As suboxide representative of the transition region at the GaAs/oxide interface are studied through density functional calculations. Two amorphous models generated by quenches from the melt are taken under consideration. The absence of As–O bonds indicates that the structure is a mixture of GaAs and Ga-oxide, in accordance with photoemission experiments. The band edges of the models are found to be closely aligned to those of GaAs. The simulation of charging and discharging processes leads to the identification of an As-related defect with an energy level at ∼0.7 eV above the GaAs valence band maximum, in good agreement with the experimental density of interface states.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗
DOE OSTI2019

Structure and reactivity of highly reduced titanium oxide surface layers on TiO 2 : A first-principles study

Titanium oxide structures featuring highly reduced TiO x films on top of nearly stoichiometric TiO 2 hold promise for applications ranging from photocatalysis to resistance switching devices. In this article, we focus on titanium monoxide (TiO) layers on anatase TiO 2 (001) and use first principles calculations to investigate their structure and properties as well as their interface with liquid water. We find that only a single TiO layer can grow epitaxially on anatase (001) and subsequent growth leads to the formation of TiO islands. The TiO layers decrease the work function and enhance the surface conductivity in comparison to pure anatase, two features that can improve the TiO 2 performance in photocatalytic hydrogen evolution but are thermodynamically unstable relative to pure TiO 2 in humid/aqueous environment. Furthermore, first principles molecular dynamics simulations of the TiO (001)-water and anatase (001)-water interfaces show that unlike the multilayer structure of interfacial water on the anatase surface, a very dense and tightly packed first water layer is present on the surface of TiO, which could represent the first stage of partial surface reoxidation.

36 MATERIALS SCIENCE↗