Global self-organization of solute induced by ion irradiation in polycrystalline alloys
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36 MATERIALS SCIENCE↗
SEARCH · Engineering Papers
Results for “surfaces interfaces and thin films”
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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Quantifying Bulk and Surface Recombination in CdTe Solar Cells Using Time-Resolved Terahertz Spectroscopy
Understanding the nature of recombination mechanisms is essential for higher power conversion efficiency in photovoltaic (PV) devices. Here we use a combination of time-resolved terahertz spectroscopy and numerical modeling to determine the bulk Shockley-Read-Hall lifetime and interface and back surface recombination velocities in CdTe thin film stacks. Furthermore, the measurement was facilitated by fabricating wire-grid device structures using conventional laser scribing. Evaluation of a glass/FTO/SnO2/CdS/CdTe stack treated with CdCl2 allowed separation of the CdTe absorber bulk lifetime, 1.6 ns, from the back surface recombination velocity, ~6x10 4 cm/s, and indicated that CdTe/CdS interface recombination velocity had no significant impact on carrier dynamics.
14 SOLAR ENERGY↗
Extending the capillary wave model to include the effect of bending rigidity: X-ray reflectivity and diffuse scattering
The surface roughness of a thin film at a liquid interface exhibits contributions of thermally excited fluctuations. This thermal roughness depends on temperature (𝑇), surface tension (𝛾), and elastic material properties, specifically the bending modulus (𝜅) of the film. A nonzero 𝜅 suppresses the thermal roughness at small length scales compared to an interface with zero 𝜅, as expressed by the power spectral density of the thermal roughness. The description of the x-ray scattering of the standard capillary wave model (CWM), which is valid for zero 𝜅, is extended to include the effect of 𝜅. The extended CWM (eCWM) provides a single analytical form for both the specular x-ray reflectivity (XRR) and the diffuse scattering around the specular reflection, and recovers the expression of the CWM at its zero 𝜅 limit. This theoretical approach enables the use of single-shot grazing incidence x-ray off-specular scattering (GIXOS) measurements for characterizing the structure of thin films on a liquid surface. The eCWM analysis approach decouples the thermal roughness factor from the surface scattering signal, providing direct access to the intrinsic surface-normal structure of the film and its bending modulus. Moreover, the eCWM facilitates the calculation of reflectivity at any desired resolution (pseudo-XRR approach). The transformation into pseudo-XRR provides the benefit of using widely available XRR software to perform GIXOS analysis. The extended range of the vertical scattering vector (𝑄 𝑧 ) available with the GIXOS pseudo-XRR approach allows for a higher spatial resolution than with conventional XRR. Experimental results are presented for various lipid systems, showing strong agreement between conventional specular XRR and pseudo-XRR methods. This agreement validates the proposed approach and highlights its utility for analyzing soft, thin films.
36 MATERIALS SCIENCE↗
Anisotropic weak antilocalization in thin films of the Weyl semimetal TaAs
Device applications of topological semimetals await the development of epitaxial films in the ultrathin limit. Weak antilocalization (WAL) has been extensively utilized in the understanding of surface states in topological insulators and shows promise for use in elucidating the properties of thin film topological semimetals. Here, we report insights from WAL in the surface state and interface transport properties of our recently synthesized single-crystal-like thin films of the Weyl semimetal TaAs(001) grown on GaAs(001). We observe robust, anisotropic WAL in the magnetoconductance from 2 to 20 K in films from 10 to 200 nm thick. We link the anisotropic WAL magnetoconductance to anisotropic mobility stemming from film topography. We conclude that WAL in the films likely originates from the antilocalization of topological surface states. The WAL magnetoconductance is impacted by the film thickness and topography, solidifying the useful role of WAL in the study of topological semimetal/semiconductor heterointerfaces. Published by the American Physical Society 2024
75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗
Application of the core shell model for strengthening polymer filament interfaces
While surface segregation has been intensively studied in thin films, relatively little has been investigated in filament geometries. In contrast to thin films, the filament surface forms a continuum, with interactions both at the free air and internal filament interface, which makes it difficult to achieve an equilibrium configuration. This asymmetry has become particularly apparent with the increasing use of additive manufacturing where entire structures are constructed via layered deposition of filamentous layers from a moving thermal nozzle. In addition, this process is highly non-equilibrated with poor thermal retention and is responsible for insufficient filament–filament interfacial fusion and internal pore formation along the printing direction. These features all contribute to poor mechanical and structural properties, which are exacerbated in semi-crystalline polymers, such as Polylactic Acid (PLA), where the melting point, T m , is much higher than the glass transition, T g . Even though system is liquid the molecules become ordered within the crystal structure and this ordering interferes with interdiffusion, which in turn prevents proper interfacial fusion. Capitalizing on the differential in surface tension, we show that addition of less than 1%, or trace amounts, of longer chain polymers, an oriented core shell structure, will be formed with a self-limiting thickness of three time the radius of gyration, R g , of the tracer chains. The lower T g of the tracers and their orientation makes them poised for interdiffusion when subsequent layers are deposited producing structures with significant improvement of the mechanical properties and internal structural integrity.
36 MATERIALS SCIENCE↗
Surface and interface structures of epitaxial Sb 2 Se 3 on mica
Sb 2 Se 3 thin film is an emerging photon absorber used in solar cells. We report the study of surface and interface structures of Sb2Se3(1 2 0) film grown on mica substrate by a high-rate vapor transport method. The interface epitaxial relationship between Sb 2 Se 3 and mica examined by the cross- sectional TEM images and diffraction patterns along the [0 0 1] and [10] directions of Sb 2 Se 3 reveal a rectangular structure with lengths of 4.03 ± 0.1 Å and 5.29 ± 0.1 Å, consistent with the [1 2 0] out-of-plane direction of Sb 2 Se 3 bulk lattice parameters. In contrast, the two-dimensional reciprocal space map (2D map) constructed from azimuthal reflection high-energy electron diffraction (ARHEED) patterns from the surface exhibits a decorated hexagonal structure. This surface structure emerges from six epitaxial orientation domains/rods and each domain has a rectangular unit mesh of 3.94 ± 0.09 Å and 26.95 ± 1.16 Å along the [0 0 1] and [10] directions. The 26.95 Å is consistent with the unit mesh of the outermost layer of the Sb 2 Se 3 (1 2 0) domains/rods. Overall, our 2D map reveals surface information that are not easily observed by other diffraction techniques.
77 NANOSCIENCE AND NANOTECHNOLOGY↗
Atomistic modeling of energy band alignment in CdTe(1 0 0) and CdTe(1 1 1) surfaces
An atomic-scale perspective of energy band alignment in CdTe surfaces has not been spatially studied despite the major role surfaces play in forming interfaces within CdTe-based thin film photovoltaic devices. Atomistic modeling based on density functional theory coupled with surface Green’s function is used for calculating energy band alignment of CdTe surfaces. The CdTe(1 0 0) ((1×1) and c(2×2) reconstruction) and CdTe(1 1 1) ((1×1) and (2×2) reconstruction) facets without and with surface relaxation provide insightful band bending characteristics that influence charge carrier transport. Results show that unrelaxed (1×1) CdTe(1 0 0) and CdTe(1 1 1) surfaces bend the valence band downward with surface polarity dictating the surface potential magnitude. The reconstructed CdTe(1 0 0) c(2×2) and CdTe(1 1 1) (2×2) surfaces result in favorable surface electronic features in relation to their unreconstructed variants. In addition, the structurally relaxed CdTe(1 1 1) surfaces develop an internal energy cusp potential that may enhance hole charge transport toward the back of CdTe solar cell devices. In conclusion, energy band alignments calculated within the study lead to a detailed understanding of how CdTe surfaces may affect CdTe-based thin film photovoltaic applications.
36 MATERIALS SCIENCE↗
Erratum: “History of atomic layer deposition and its relationship with the American Vacuum Society” [J. Vac. Sci. Technol. A 31, 050818 (2013)]
The authors of this review article published in 20131 would like to correct some text and references relating to the first observations and publications on molecular layering. In Sec. II, “Early Years of Atomic Layer Processes” in the original article,1 the first two sentences of the fourth paragraph should instead say “The ALD principle, where surface reactions follow a binary sequence of self-limiting half-reactions, was reported under the name ‘molecular layering’ in the 1960s by S. I. Kol’tsov from Leningrad Technological Institute.2–6 These experiments were conducted under the scientific supervision of V. B. Aleskovskii. The ‘framework hypothesis,’ an antecedent to molecular layering, was proposed by V. B. Aleskovskii in 1952.6” In addition, again in this same section and paragraph, the last two sentences should instead say “In the 1969 article,3 the authors report that the initial reaction between TiCl4 and Si–OH tends to involve 3 Si–OH, forming one Ti–Cl, whereas after the first water step, the second TiCl4 exposure reacts with 2 Ti–OH, forming Ti–Cl2 groups. In the 1969 paper,3 a planar thin film was not produced or evaluated, although nanolayers were prepared by molecular layering at that time.6” These corrections do not affect other sections or the conclusions drawn in the article.
37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
Phonon confinement and interface lattice dynamics of ultrathin high- k rare earth sesquioxide films: the case of Eu 2 O 3 on YSZ(001)
The spatial confinement of atoms at surfaces and interfaces significantly alters the lattice dynamics of thin films, heterostructures and multilayers. Ultrathin films with high dielectric constants (high-k) are of paramount interest for applications as gate layers in current and future integrated circuits. Here we report a lattice dynamics study of high-k Eu 2 O 3 films with thicknesses of 21.3, 2.2, 1.3, and 0.8 nm deposited on YSZ(001). The Eu-partial phonon density of states (PDOS), obtained from nuclear inelastic scattering, exhibits broadening of the phonon peaks accompanied by up to a four-fold enhancement of the number of low-energy states compared to the ab initio calculated PDOS of a perfect Eu 2 O 3 crystal. Our analysis demonstrates that while the former effect reflects the reduced phonon lifetimes observed in thin films due to scattering from lattice defects, the latter phenomenon arises from an ultrathin EuO layer formed between the thin Eu 2 O 3 film and the YSZ(001) substrate. Thus, our work uncovers another potential source of vibrational anomalies in thin films and multilayers, which has to be cautiously considered.
37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
Bias‐Dependent Quantum Efficiency Reveals Recombination Pathways in Thin Film Solar Cells
Identifying where recombination predominantly occurs—whether at the front interface, back interface, or throughout the bulk—is crucial for optimizing CdSeTe solar cells and many other photovoltaic device architectures. Here, a simple and effective diagnostic is demonstrated: measuring external quantum efficiency (QE) under varying forward biases. The drift–diffusion simulations reveal that each recombination pathway leaves a distinct bias-induced signature in the normalized QE: a progressive drop at long wavelengths for back-limited devices, a short-wavelength decline for front-limited devices, and a relatively uniform decrease across all wavelengths for bulk-limited devices. These predictions are validated with experiments on As-doped and Cu-doped CdSeTe devices, with and without passivation layers or different front buffers. In each case, the observed bias-dependent QE spectral changes align with the simulated recombination map. Because this method uses standard QE instrumentation, it offers a broadly accessible and cost-efficient means to diagnose recombination pathways—extending beyond CdSeTe to other thin-film and emerging solar cell technologies. By pinpointing recombination bottlenecks, researchers and manufacturers can strategically refine doping profiles, passivation schemes, and interface designs to further improve device performance.
CdTe↗
Increase in the effective viscosity of polyethylene under extreme nanoconfinement
Understanding polymer transport in nanopores is crucial for optimizing heterogeneously catalyzed processes in polymer upcycling and fabricating high-performance nanocomposite films and membranes. Although confined polymer dynamics have been extensively studied, the behavior of polyethylene (PE)—the most widely used commodity polymer—in pores smaller than 20 nm remains largely unexplored. We investigate the effects of extreme nanoconfinement on PE transport using capillary rise infiltration in silica nanoparticle packings with average pore radii ranging from ~1 to ~9 nm. Using in situ ellipsometry and the Lucas–Washburn model, we discover a previously unknown inverse relationship between effective viscosity (η eff ) and average pore radius (R pore ). Additonally, we determine that PE transport under these extreme conditions is primarily governed by physical confinement, rather than pore surface chemistry. We refine an existing theory to provide a generalized formalism to describe the polymer transport dynamics over a wide range of pore radii (from 1 nm and larger). Our results offer valuable insights for optimizing catalyst supports in polymer upcycling and improving infiltration processes for nanocomposite fabrication.
36 MATERIALS SCIENCE↗
Purely electronic insulator-metal transition in rutile VO 2
Volatile resistive switching in neuromorphic computing can be tuned by external stimuli such as temperature or electric-field. However, this type of switching is generally coupled to structural changes, resulting in slower reaction speed and higher energy consumption when incorporated into an electronic device. The vanadium dioxide (VO 2 ), which has near room temperature metal-insulator transition (MIT), is an archetypical volatile resistive switching system. Here, we demonstrate an isostructural MIT in an ultrathin VO 2 film capped with a photoconductive cadmium sulfide (CdS) layer. Transmission electron microscopy, resistivity experiments, and first-principles calculations show that the hole carriers induced by CdS photovoltaic effect are driving the MIT in rutile VO 2 . The insulating-rutile VO 2 phase has been proved and can remain stable for hours. Our finding provides a new approach to produce purely electronically driven MIT in VO 2 , and widens its applications in fast-response, low-energy neuromorphic devices.
75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗
Experimental observation of localized interfacial phonon modes
Interfaces impede heat flow in micro/nanostructured systems. Conventional theories for interfacial thermal transport were derived based on bulk phonon properties of the materials making up the interface without explicitly considering the atomistic interfacial details, which are found critical to correctly describing thermal boundary conductance. Recent theoretical studies predicted the existence of localized phonon modes at the interface which can play an important role in understanding interfacial thermal transport. However, experimental validation is still lacking. Through a combination of Raman spectroscopy and high-energy-resolution electron energy-loss spectroscopy in a scanning transmission electron microscope, we report the experimental observation of localized interfacial phonon modes at ~12 THz at a high-quality epitaxial Si-Ge interface. These modes are further confirmed using molecular dynamics simulations with a high-fidelity neural network interatomic potential, which also yield thermal boundary conductance agreeing well with that measured in time-domain thermoreflectance experiments. Simulations find that the interfacial phonon modes have an obvious contribution to the total thermal boundary conductance. Our findings significantly contribute to the understanding of interfacial thermal transport physics and have impact on engineering thermal boundary conductance at interfaces in applications such as electronics thermal management and thermoelectric energy conversion.
36 MATERIALS SCIENCE↗
Complexions at the iron-magnetite interface
Synthesizing distinct phases and controlling crystalline defects are key concepts in materials design. These approaches are often decoupled, with the former grounded in equilibrium thermodynamics and the latter in nonequilibrium kinetics. By unifying them through defect phase diagrams, we can apply phase equilibrium models to thermodynamically evaluate defects—including dislocations, grain boundaries, and phase boundaries—establishing a theoretical framework linking material imperfections to properties. Using scanning transmission electron microscopy (STEM) with differential phase contrast (DPC) imaging, we achieve the simultaneous imaging of heavy Fe and light O atoms, precisely mapping the atomic structure and chemical composition at the iron-magnetite (Fe/Fe 3 O 4 ) interface. We identify a well-ordered two-layer interface-stabilized phase state (referred to as complexion) at the Fe[001]/Fe 3 O 4 [001] interface. Using density-functional theory (DFT), we explain the observed complexion and map out various interface-stabilized phases as a function of the O chemical potential. The formation of complexions increases interface adhesion by 20% and alters charge transfer between adjacent materials, impacting transport properties. Our findings highlight the potential of tunable defect-stabilized phase states as a degree of freedom in materials design, enabling optimized corrosion protection, catalysis, and redox-driven phase transitions, with applications in materials sustainability, efficient energy conversion, and green steel production.
36 MATERIALS SCIENCE↗
Light-field control of real and virtual charge carriers
We report light-driven electronic excitation is a cornerstone for energy and information transfer. In the interaction of intense and ultrafast light fields with solids, electrons may be excited irreversibly, or transiently during illumination only. As the transient electron population cannot be observed after the light pulse is gone, it is referred to as virtual, whereas the population that remains excited is called real. Virtual charge carriers have recently been associated with high-harmonic generation and transient absorption, but photocurrent generation may stem from real as well as virtual charge carriers. However, a link between the generation of the carrier types and their importance for observables of technological relevance is missing. Here we show that real and virtual charge carriers can be excited and disentangled in the optical generation of currents in a gold–graphene–gold heterostructure using few-cycle laser pulses. Depending on the waveform used for photoexcitation, real carriers receive net momentum and propagate to the gold electrodes, whereas virtual carriers generate a polarization response read out at the gold–graphene interfaces. On the basis of these insights, we further demonstrate a proof of concept of a logic gate for future lightwave electronics. Our results offer a direct means to monitor and excite real and virtual charge carriers. Individual control over each type of carrier will markedly increase the integrated-circuit design space and bring petahertz signal processing closer to reality.
72 PHYSICS OF ELEMENTARY PARTICLES AND FIELDS↗
Nanoscale imaging of phonon dynamics by electron microscopy
Spatially resolved vibrational mapping of nanostructures is indispensable to the development and understanding of thermal nanodevices, modulation of thermal transport and novel nanostructured thermoelectric materials. Through the engineering of complex structures, such as alloys, nanostructures and superlattice interfaces, one can significantly alter the propagation of phonons and suppress material thermal conductivity while maintaining electrical conductivity. There have been no correlative experiments that spatially track the modulation of phonon properties in and around nanostructures due to spatial resolution limitations of conventional optical phonon detection techniques. Here we demonstrate two-dimensional spatial mapping of phonons in a single silicon–germanium (SiGe) quantum dot (QD) using monochromated electron energy loss spectroscopy in the transmission electron microscope. Tracking the variation of the Si optical mode in and around the QD, we observe the nanoscale modification of the composition-induced red shift. We observe non-equilibrium phonons that only exist near the interface and, furthermore, develop a novel technique to differentially map phonon momenta, providing direct evidence that the interplay between diffuse and specular reflection largely depends on the detailed atomistic structure: a major advancement in the field. Our work unveils the non-equilibrium phonon dynamics at nanoscale interfaces and can be used to study actual nanodevices and aid in the understanding of heat dissipation near nanoscale hotspots, which is crucial for future high-performance nanoelectronics.
36 MATERIALS SCIENCE↗
Elucidating the water–anatase TiO 2 (101) interface structure using infrared signatures and molecular dynamics
The structure and dynamics of water on solid surfaces critically affect the chemistry of materials in ambient and aqueous environments. Here, we investigate the hydrogen bonding network of water adsorbed on the majority (101) surface of anatase TiO 2 , a widely used photocatalyst, using polarization- and azimuth-resolved infrared spectroscopy combined with neural network potential molecular dynamics simulations. Our results show that one monolayer of water saturates the undercoordinated titanium (Ti 5c ) sites, forming one-dimensional chains of molecule hydrogen bonded to surface undercoordinated bridging oxygen (O 2c ) atoms. As the coverage increases, water adsorption on O 2c sites leads to significant restructuring of the water monolayer and the formation of a two-dimensional hydrogen bond network characterized by tightly bound pairs of water molecules on adjacent Ti 5c and O 2c sites. This structural motif likely persists at ambient conditions, influencing the reactions occurring there. In conclusion, the results reported here provide critical details of the structure of the water–anatase (101) interface that were previously hypothesized but unconfirmed experimentally.
37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
Reducing Non-Radiative Recombination in Perovskite Solar Cells with a SiO2-Graphene Oxide Buried Interface Layer
Perovskite solar cells (PSCs) have emerged as a transformative photovoltaic technology. However, the device performance of inverted PSCs is dramatically limited by surface defects and the underlying film morphology of metal halide perovskite (MHP) thin film. Herein, we report a novel buried interface layer consisting of SiO2 nanoparticles (NPs) chemically bonded to graphene oxide (GO), deposited atop a hydrophobic hole extraction layer (HEL) to address this limitation. The SiO2 NPs serve as insoluble scaffolds that immobilize GO sheets on the hydrophobic HEL surface, enabling the formation of homogeneous MHP thin films. Meanwhile, the GO functional groups interact with surface-uncoordinated Pb2+, suppressing interfacial defects and guiding crystal grain growth of the resultant MHP thin films. This synergistic effect suppresses non-radiative charge recombination and enhances charge extraction efficiency. As a result, a 26.07% efficiency with significantly suppressed photocurrent hysteresis is observed from PSCs incorporating the SiO2-GO buried interface layer. Moreover, the above PSCs maintain 92% of their initial PCE after 1800 h of continuous operation at the maximum power point under AM 1.5 G (100 mW/cm2) illumination at 25 degrees C in air with 50-60% relative humidity. These results demonstrate that we have developed a facile and effective way to realize high-performance inverted PSCs.
14 SOLAR ENERGY↗