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At least 1,315 records · Page 73

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DOE OSTI2013

Improved passivation of the ZnO/Si interface by pulsed laser deposition

Zinc oxide thin-films were grown on crystalline silicon employing magnetron sputtering and pulsed laser deposition. Bulk and interface properties were investigated using scanning electron microscopy, Raman backscattering, photoluminescence, and infrared spectroscopic ellipsometry. Sputter deposited ZnO samples reveal a large degree of disorder and an interface defect density of Almost-Equal-To 10{sup 12} cm{sup -2}. A significant improvement of the structural quality is observed in samples grown by pulsed laser deposition. The bulk defect density is further reduced, when introducing monatomic oxygen during deposition. Simultaneously, the defect density at the ZnO/Si interface decreases by about a factor of five. Implications for devices containing ZnO/Si interfaces are discussed.

36 MATERIALS SCIENCE↗

DOE OSTI2013

Conducting and insulating LaAlO{sub 3}/SrTiO{sub 3} interfaces: A comparative surface photovoltage investigation

Surface photovoltage (SPV) spectroscopy, which is a versatile method to analyze the energetic distribution of electronic defect states at surfaces and interfaces of wide-bandgap semiconductor (hetero-)structures, is applied to comparatively investigate heterostructures made of 5-unit-cell-thick LaAlO{sub 3} films grown either on TiO{sub 2}- or on SrO-terminated SrTiO{sub 3}. As shown in a number of experimental and theoretical investigations in the past, these two interfaces exhibit dramatically different properties with the first being conducting and the second insulating. Our present SPV investigation reveals clearly distinguishable interface defect state distributions for both configurations when interpreted within the framework of a classical semiconductor band scheme. Furthermore, bare SrTiO{sub 3} crystals with TiO{sub 2} or mixed SrO/TiO{sub 2} terminations show similar SPV spectra and transients as do LaAlO{sub 3}-covered samples with the respective termination of the SrTiO{sub 3} substrate. This is in accordance with a number of recent works that stress the decisive role of SrTiO{sub 3} and the minor role of LaAlO{sub 3} with respect to the electronic interface properties.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗

DOE OSTI2014

Valence and conduction band offsets at amorphous hexagonal boron nitride interfaces with silicon network dielectrics

To facilitate the design of heterostructure devices employing hexagonal/sp{sup 2} boron nitride, x-ray photoelectron spectroscopy has been utilized in conjunction with prior reflection electron energy loss spectroscopy measurements to determine the valence and conduction band offsets (VBOs and CBOs) present at interfaces formed between amorphous hydrogenated sp{sup 2} boron nitride (a-BN:H) and various low- and high-dielectric-constant (k) amorphous hydrogenated silicon network dielectric materials (a-SiX:H, X = O, N, C). For a-BN:H interfaces formed with wide-band-gap a-SiO{sub 2} and low-k a-SiOC:H materials (E{sub g} ≅ 8.2−8.8 eV), a type I band alignment was observed where the a-BN:H band gap (E{sub g} = 5.5 ± 0.2 eV) was bracketed by a relatively large VBO and CBO of ∼1.9 and 1.2 eV, respectively. Similarly, a type I alignment was observed between a-BN:H and high-k a-SiC:H where the a-SiC:H band gap (E{sub g} = 2.6 ± 0.2 eV) was bracketed by a-BN:H with VBO and CBO of 1.0 ± 0.1 and 1.9 ± 0.2 eV, respectively. The addition of O or N to a-SiC:H was observed to decrease the VBO and increase the CBO with a-BN:H. For high-k a-SiN:H (E{sub g} = 3.3 ± 0.2 eV) interfaces with a-BN:H, a slightly staggered type II band alignment was observed with VBO and CBO of 0.1 ± 0.1 and −2.3 ± 0.2 eV, respectively. The measured a-BN:H VBOs were found to be consistent with those deduced via application of the commutative and transitive rules to VBOs reported for a-BN:H, a-SiC:H, a-SiN:H, and a-SiO{sub 2} interfaces with Si (100)

36 MATERIALS SCIENCE↗

DOE OSTI2014

Stacking faults and interface roughening in semipolar (202{sup ¯}1{sup ¯}) single InGaN quantum wells for long wavelength emission

The microstructure of InGaN single quantum wells (QWs) grown in semipolar (202{sup ¯}1{sup ¯}) orientation on GaN substrates was studied by transmission electron microscopy. Stress relaxation in the lattice mismatch In{sub x}Ga{sub 1−x}N layer was realized by forming partial misfit dislocations associated with basal plane stacking faults (BPSFs). For given composition x = 0.24, BPSFs formation was observed when the QW thickness exceeded 4 nm. The high density of partial threading dislocations that bound the BPSFs is detrimental to light-emitting device performance. Interface roughening (faceting) was observed for both upper and lower QW interfaces (more pronounced for upper interface) and was found to increase with the thickness of the QW. BPSFs had a tendency to nucleate at roughened interface valleys.

36 MATERIALS SCIENCE↗

DOE OSTI2014

Fullerene film on metal surface: Diffusion of metal atoms and interface model

We try to understand the fact that fullerene film behaves as n-type semiconductor in electronic devices and establish a model describing the energy level alignment at fullerene/metal interfaces. The C{sub 60}/Ag(100) system was taken as a prototype and studied with photoemission measurements. The photoemission spectra revealed that the Ag atoms of the substrate diffused far into C{sub 60} film and donated electrons to the molecules. So the C{sub 60} film became n-type semiconductor with the Ag atoms acting as dopants. The C{sub 60}/Ag(100) interface should be understood as two sub-interfaces on both sides of the molecular layer directly contacting with the substrate. One sub-interface is Fermi level alignment, and the other is vacuum level alignment.

36 MATERIALS SCIENCE↗

DOE OSTI2016

Density functional theory based study of chlorine doped WS{sub 2}-metal interface

Investigation of a transition metal dichalcogenide (TMD)-metal interface is essential for the effective functioning of monolayer TMD based field effect transistors. In this work, we employ the Density Functional Theory calculations to analyze the modulation of the electronic structure of monolayer WS{sub 2} with chlorine doping and the relative changes in the contact properties when interfaced with gold and palladium. We initially examine the atomic and electronic structures of pure and doped monolayer WS{sub 2} supercell and explore the formation of midgap states with band splitting near the conduction band edge. Further, we analyze the contact nature of the pure supercell with Au and Pd. We find that while Au is physiosorbed and forms n-type contact, Pd is chemisorped and forms p-type contact with a higher valence electron density. Next, we study the interface formed between the Cl-doped supercell and metals and observe a reduction in the Schottky barrier height (SBH) in comparison to the pure supercell. This reduction found is higher for Pd in comparison to Au, which is further validated by examining the charge transfer occurring at the interface. Our study confirms that Cl doping is an efficient mechanism to reduce the n-SBH for both Au and Pd, which form different types of contact with WS{sub 2}.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗

DOE OSTI2017

Energy level alignment at molecule-metal interfaces from an optimally tuned range-separated hybrid functional

The alignment of the frontier orbital energies of an adsorbed molecule with the substrate Fermi level at metal-organic interfaces is a fundamental observable of significant practical importance in nanoscience and beyond. Typical density functional theory calculations, especially those using local and semi-local functionals, often underestimate level alignment leading to inaccurate electronic structure and charge transport properties. Here, we develop a new fully self-consistent predictive scheme to accurately compute level alignment at certain classes of complex heterogeneous molecule-metal interfaces based on optimally tuned range-separated hybrid functionals. Starting from a highly accurate description of the gas-phase electronic structure, our method by construction captures important nonlocal surface polarization effects via tuning of the long-range screened exchange in a range-separated hybrid in a non-empirical and system-specific manner. We implement this functional in a plane-wave code and apply it to several physisorbed and chemisorbed molecule-metal interface systems. Our results are in quantitative agreement with experiments, the both the level alignment and work function changes. This approach constitutes a new practical scheme for accurate and efficient calculations of the electronic structure of molecule-metal interfaces.

36 MATERIALS SCIENCE↗

DOE OSTI2017

Fast ion transport at a gas-metal interface

Fast ion transport and the resulting fusion yield reduction are computed at a gas-metal interface. The extent of fusion yield reduction is observed to depend sensitively on the charge state of the surrounding pusher material and the width of the atomically mixed region. These sensitivities suggest that idealized boundary conditions often implemented at the gas-pusher interface for the purpose of estimating fast ion loss will likely overestimate fusion reactivity reduction in several important limits. Additionally, the impact of a spatially complex material interface is investigated by considering a collection of droplets of the pusher material immersed in a DT plasma. It is found that for small Knudsen numbers, the extent of fusion yield reduction scales with the surface area of the material interface. As the Knudsen number is increased, but, the simple surface area scaling is broken, suggesting that hydrodynamic mix has a nontrivial impact on the extent of fast ion losses.

70 PLASMA PHYSICS AND FUSION TECHNOLOGY↗

DOE OSTI2017

Direct imaging of sketched conductive nanostructures at the LaAlO 3 /SrTiO 3 interface

Nanoscale control of the quasi-two-dimensional electron gas at the LaAlO 3 /SrTiO 3 (LAO/STO) interface by a conductive probe tip has triggered the development of a number of electronic devices. While the spatial distribution of the conductance is crucial for such devices, it is challenging to directly visualize the local electrical properties at the buried interface. Here, we demonstrate conductivity imaging of sketched nanostructures at the LAO/STO interface by microwave impedance microscopy (MIM) with a lateral resolution on the order of 100 nm. The sheet conductance extracted from the MIM data agrees with the transport measurement. The tip-induced insulator-to-metal transition is observed above a threshold voltage of +4 V. Our work paves the way for studying emergent phenomena at oxide interfaces by probing nanoscale conductance distribution.

36 MATERIALS SCIENCE↗

DOE OSTI2018

The stability of the contact interface of cylindrical and spherical shock tubes

The stability of the contact interface for radial shock tubes is investigated as a model for explosive dispersal. The advection upstream splitting method with velocity and pressure diffusion (AUSM+-up) is used to solve for the radial base flow. To explore the stability of the resulting contact interface, perturbed governing equations are derived assuming harmonic modes in the transverse directions. The perturbed harmonic flow is solved by assuming an initial disturbance and using a perturbed version of AUSM+-up derived in this paper. The intensity of the perturbation near the contact interface is computed and compared to theoretical results obtained by others. Despite the simplifying assumptions of the theoretical analysis, very good agreement is confirmed. Not only can the magnitude of the instability be predicted during the initial expansion, but also remarkably the agreement between the numerical and theoretical results can be maintained through the collision between the secondary shock and the contact interface. Since the theoretical results only depend upon the time evolution of the base flow, the stability of various modes could be quickly studied without explicitly solving a system of partial differential equations for the perturbed flow.

42 ENGINEERING↗

DOE OSTI2019

Modulating electronic coupling at the quantum dot/molecule interface by wavefunction engineering

In this work, we use wavefunction engineering by varying the size of Quantum Dots (QDs) and tuning the delocalization (or diffuseness) of frontier orbitals of an acceptor molecule to modulate charge transfer dynamics at the QD/molecule interface. For this purpose, we apply our recently developed bulk-adjusted linear combination of atomic orbitals (BA-LCAO) approach for nanostructures and a density functional theory (DFT) for the acceptor molecules. These electronic structure calculations, combined with extensive molecular dynamics simulations using a fragmented molecular mechanics (FraMM) force field, reveal intimate details of charge transfer across the QD/Acceptor interface. For the spherical wurtzite-(CdSe) 201 and (CdSe) 693 nanostructures, as model QDs with respective 2.8 and 4.1 nm diameters, and anthraquinone-2,3-dicarboxylic acid and its derivatives with the 7-OH, 7-OF, 10-BH, and 10-CH 2 substituents, as model molecular acceptors, we find that (1) both the electron donating and withdrawing groups greatly enhance hole transfer by means of diffusing the acceptor HOMO; (2) electron transfer is affected only by the electron donating groups; (3) solvent effects are largely negligible for the orbital overlaps, and (4) consistent with spatial confinement theories, the electron density of the smaller QD penetrates farther into the vacuum than the corresponding density of the larger QD leading to stronger coupling with the acceptor. These findings suggest that (a) one can effectively control charge transfer across the QD/molecule interface by either changing the size of the QD or by tuning diffuseness of frontier orbitals of the acceptor molecule and (b) the combination of the recently developed BA-LCAO approach for QDs with a DFT for the acceptor molecules, facilitated by the use of the FraMM force field and extensive molecular dynamics simulations, provide qualitatively accurate description of charge transfer dynamics at the QD/acceptor interface.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

DOE OSTI2019

Determining interface structures in vertically aligned nanocomposite films

Vertically aligned nanocomposites (VANs) films have self-assembled pillar-matrix nanostructures. Owing to their large area-to-volume ratios, interfaces in VAN films are expected to play key roles in inducing functional properties, but our understanding is hindered by limited knowledge about their structures. Motivated by the lack of definitive explanation for the experimentally-found enhanced ionic conductivity in Sm-doped-Ce0 2 /SrTiO 3 VAN films, we determine the structure at vertical interfaces using random structure searching and explore how it can affect ionic conduction. Interatomic potentials are used to perform the initial searching, followed by firstprinciples calculations for refinement. Previously unknown structures are found, with lower energy than that of an optimized hand-built model. We find a strongly distorted oxygen sub-lattice which gives a complex landscape of vacancy energies. The cation lattice remains similar to the bulk phase, but has a localized strain field. The excess energy of the interface is similar to that of a high angle grain boundaries in SrTiO 3 . None of the observations supports ionic conductivity being enhanced locally at the interface.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗

DOE OSTI2020

An in situ shearing x-ray measurement system for exploring structures and dynamics at the solid–liquid interface

Revealing interfacial structure and dynamics has been one of the essential thematic topics in material science and condensed matter physics. Synchrotron-based x-ray scattering techniques can deliver unique and insightful probing of interfacial structures and dynamics, in particular, in reflection geometries with higher surface and interfacial sensitivity than transmission geometries. We demonstrate the design and implementation of an in situ shearing x-ray measurement system, equipped with both inline parallel-plate and cone-and-plate shearing setups and operated at the advanced photon source at Argonne National Laboratory, to investigate the structures and dynamics of end-tethered polymers at the solid-liquid interface. With a precise lifting motor, a micrometer-scale gap can be produced by aligning two surfaces of a rotating upper shaft and a lower sample substrate. A torsional shear flow forms in the gap and applies tangential shear forces on the sample surface. The technical combination with nanoscale rheology and the utilization of in situ x-ray scattering allow us to gain fundamental insights into the complex dynamics in soft interfaces under shearing. In this work, we demonstrate the technical scope and experimental capability of the in situ shearing x-ray system through the measurements of charged polymers at both flat and curved interfaces upon shearing. Furthermore, through the in situ shearing x-ray scattering experiments integrated with theoretical simulations, we aim to develop a detailed understanding of the short-range molecular structure and mesoscale ionic aggregate morphology, as well as ion transport and dynamics in soft interfaces, thereby providing fundamental insight into a long-standing challenge in ionic polymer brushes with a significant technological impact.

36 MATERIALS SCIENCE↗

DOE OSTI2021

Synchrotron studies of functional interfaces and the state of the art: A perspective

The dramatic improvements in synchrotron light sources across the world imply tremendous opportunities for interface science. In this work, we describe a variety of current scattering and spectroscopic techniques with an eye toward how these will evolve, particularly with the advent of diffraction-limited sources. We also note the importance of in situ and operando methods for both understanding interface creation and interface evolution in different environments. As interfaces are often where critical processes occur, whether in regard to energy/chemical/materials/quantum information science, understanding the utility of these x-ray techniques will be of considerable importance to the cultivation of next-generation scientists.

36 MATERIALS SCIENCE↗

DOE OSTI2021

AENET–LAMMPS and AENET–TINKER : Interfaces for accurate and efficient molecular dynamics simulations with machine learning potentials

Machine-learning potentials (MLPs) trained on data from quantum-mechanics based first-principles methods can approach the accuracy of the reference method at a fraction of the computational cost. To facilitate efficient MLP-based molecular dynamics and Monte Carlo simulations, an integration of the MLPs with sampling software is needed. Here, we develop two interfaces that link the atomic energy network (ænet) MLP package with the popular sampling packages TINKER and LAMMPS. The three packages, ænet, TINKER, and LAMMPS, are free and open-source software that enable, in combination, accurate simulations of large and complex systems with low computational cost that scales linearly with the number of atoms. Scaling tests show that the parallel efficiency of the ænet–TINKER interface is nearly optimal but is limited to shared-memory systems. The ænet–LAMMPS interface achieves excellent parallel efficiency on highly parallel distributed memory systems and benefits from the highly optimized neighbor list implemented in LAMMPS. We demonstrate the utility of the two MLP interfaces for two relevant example applications: the investigation of diffusion phenomena in liquid water and the equilibration of nanostructured amorphous battery materials.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

DOE OSTI2022

Polar liquids at charged interfaces: A dipolar shell theory

The structure of polar liquids and electrolytic solutions, such as water and aqueous electrolytes, at interfaces underlies numerous phenomena in physics, chemistry, biology, and engineering. In this work, we develop a continuum theory that captures the essential features of dielectric screening by polar liquids at charged interfaces, including decaying spatial oscillations in charge and mass, starting from the molecular properties of the solvent. The theory predicts an anisotropic dielectric tensor of interfacial polar liquids previously studied in molecular dynamics simulations. We explore the effect of the interfacial polar liquid properties on the capacitance of the electrode/electrolyte interface and on hydration forces between two plane-parallel polarized surfaces. In the linear response approximation, we obtain simple formulas for the characteristic decay lengths of molecular and ionic profiles at the interface.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

DOE OSTI2023

Trap passivation of 4H-SiC/SiO 2 interfaces by nitrogen annealing

We report an N 2 based annealing treatment to passivate interface traps (D it ) in n- and p-type 4H-SiC. The process has the potential to replace the commonly used hazardous and expensive gas nitric oxide (NO). N 2 postoxidation annealing reduces D it in both the upper and lower halves of the 4H-SiC bandgap, with a greater impact at the valence band edge. N 2 annealing at 1500 °C is observed to be more effective in passivating traps and positive fixed charges than NO annealing for p-type devices, whereas for n-type devices, the opposite is true. The breakdown voltages for these devices are found to be lower than that of NO annealed devices. X-ray photoelectron spectroscopy has been performed to estimate the nitrogen areal density at the interface. D it is measured as a function of nitrogen areal densities in the near interfacial regions for the different processes. Additionally, theoretical analysis through density functional theory is consistent with the measured D it profiles by showing the generation of additional states near the valence band edge due to increased nitrogen concentration. In addition to reporting the effect of N 2 annealing on both n- and p-type 4H-SiC, this work correlates the nitrogen areal densities at the interface to the D it and explains the difference in D it characteristics with nitrogen areal density between n- and p-type interfaces.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

DOE OSTI2024

Interface-modulated kinetic differentials in electron and hole transfer rates as a key design principle for redox photocatalysis by Sb2VO5/QD heterostructures

The efficient conversion of solar energy to chemical energy represents a critical bottleneck to the energy transition. Photocatalytic splitting of water to generate solar fuels is a promising solution. Semiconductor quantum dots (QDs) are prime candidates for light-harvesting components of photocatalytic heterostructures, given their size-dependent photophysical properties and band-edge energies. A promising series of heterostructured photocatalysts interface QDs with transition-metal oxides which embed midgap electronic states derived from the stereochemically active electron lone pairs of p-block cations. Here, we examine the thermodynamic driving forces and dynamics of charge separation in Sb2VO5/CdSe QD heterostructures, wherein a high density of Sb 5s2-derived midgap states are prospective acceptors for photogenerated holes. Hard-x-ray valence band photoemission spectroscopy measurements of Sb2VO5/CdSe QD heterostructures were used to deduce thermodynamic driving forces for charge separation. Interfacial charge transfer dynamics in the heterostructures were examined as a function of the mode of interfacial connectivity, contrasting heterostructures with direct interfaces assembled by successive ion layer adsorption and reaction (SILAR) and interfaces comprising molecular bridges assembled by linker-assisted assembly (LAA). Transient absorption spectroscopy measurements indicate ultrafast (<2 ps) electron and hole transfer in SILAR-derived heterostructures, whereas LAA-derived heterostructures show orders of magnitude differentials in the kinetics of hole (<100 ps) and electron (∼1 ns) transfer. The interface-modulated kinetic differentials in electron and hole transfer rates underpin the more effective charge separation, reduced charge recombination, and greater photocatalytic efficiency observed for the LAA-derived Sb2VO5/CdSe QD heterostructures.

Chemistry↗