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At least 163 records · Page 9

Local impedance measurement of an electrode/single-pentacene-grain interface by frequency-modulation scanning impedance microscopy

The device performances of organic thin film transistors are often limited by the metal–organic interface because of the disordered molecular layers at the interface and the energy barriers against the carrier injection. It is important to study the local impedance at the interface without being affected by the interface morphology. We combined frequency modulation atomic force microscopy with scanning impedance microscopy (SIM) to sensitively measure the ac responses of the interface to an ac voltage applied across the interface and the dc potential drop at the interface. By using the frequency-modulation SIM (FM-SIM) technique, we characterized the interface impedance of a Pt electrode and a single pentacene grain as a parallel circuit of a contact resistance and a capacitance. We found that the reduction of the contact resistance was caused by the reduction of the energy level mismatch at the interface by the FM-SIM measurements, demonstrating the usefulness of the FM-SIM technique for investigation of the local interface impedance without being affected by its morphology.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗

Buffer/absorber interface recombination reduction and improvement of back-contact barrier height in CdTe solar cells

Electronic properties of a CdTe solar cell are reported using temperature-dependent capacitance spectroscopy and current-voltage characteristics, the latter in dark and illuminated conditions. The baseline solar cell material stack investigated is comprised of soda-lime-glass/SnO 2 :F/SnO 2 /CdS:O-buffer/CdTe-absorber/Cu/Au. Properties are compared with CdTe solar cells in which the back surface was hydroiodic acid etched, before the back-contact formation, and a CdTe device in which Mg-doped ZnO (MZO) replaces buffer layer CdS. Reduced back-contact barrier height and grain boundary barrier height are observed in the HI treated CdTe cell. As a result, improved device performance in the MZO-based CdTe device is attributed to reduced emitter/absorber interface recombination when using the MZO window layer.

14 SOLAR ENERGY↗

Temperature dependent interfacial microstructure in HIP-bonded Al6061/Zr joints

Pressing (HIP) at 450 °C and 560 °C under 103 MPa for 90 minutes to evaluate interfacial diffusion and microstructural evolution. Sound metallurgical bonding was achieved at both temperatures, with Zr serving as an effective diffusion barrier. Microstructural analysis revealed the the formation of a (Al,Si)3Zr intermetallic layer at the Al/Zr interface, whose thickness increased from ~100 nm at 450 °C to ~2100 nm at 560 °C, consistent with temperature-driven diffusion kinetics. The thin and continuous reaction layer observed at 450 °C indicates controlled interdiffusion and minimal reaction zone growth, favorable for maintaining interface stability and ductility. At 560 °C, enhanced atomic mobility led to pronounced intermetallic development, confirming diffusion-controlled growth behavior. These results provide valuable insights for optimizing Al/Zr interface design and diffusion barrier performance in advanced structural and energy systems.

Al/Zr interface↗

An XPS study of silicon/noble metal interfaces - Bonding trends and correlations with the Schottky barrier heights

This X-ray photoemission (XPS) study demonstrates a correlation of intrinsic TM-Si chemical bond formation with Schottky barrier heights for the near-noble transition metals (TM = Ni, Pd, Pt) and their corresponding silicides (TM2Si and TMSi) on Si(100). It is found that the barrier height correlates with the strength of the TM-Si orbital interaction as well as with the charge density around the Si atom. These observations suggest a dominant role for intrinsic chemical interactions in establishing the Schottky barrier heights in these TM-Si systems.

Grunthaner, P. J.↗

Accretion of Gas Giants Constrained by the Tidal Barrier

After protoplanets have acquired sufficient mass to open partial gaps in their natal protostellar disks, residual gas continues to diffuse onto horseshoe streamlines under the effect of viscous dissipation, and to meander in and out of the planets' Hill sphere. Within the Hill sphere, the horseshoe streamlines intercept gas flow in circumplanetary disks. The host star's tidal perturbation induces a barrier across the converging streamlines' interface. Viscous transfer of angular momentum across this tidal barrier determines the rate of mass diffusion from the horseshoe streamlines onto the circumplanetary disks, and eventually the accretion rate onto the protoplanets. Here, we carry out a series of numerical simulations to test the influence of this tidal barrier on superthermal planets. In weakly viscous disks, the protoplanets' accretion rate steeply decreases with their masses above the thermal limit. As their growth timescale exceeds the gas depletion timescale, their masses reach asymptotic values comparable to that of Jupiter. In relatively thick and strongly viscous disks, protoplanets' asymptotic masses exceed several times that of Jupiter. Two-dimensional numerical simulations show that such massive protoplanets strongly excite the eccentricity of nearby horseshoe streamlines, destabilize orderly flow, substantially enhance the diffusion rate across the tidal barrier, and elevate their growth rate until their natal disk is severely depleted. In contrast, eccentric streamlines remain stable in three-dimensional simulations. Based on the upper falloff in the observed mass distribution of known exoplanets, we suggest that their natal disks had relatively low viscosity (α ~ 10 –3 ) and modest thickness (H/R ~ 0.03–0.05).

79 ASTRONOMY AND ASTROPHYSICS↗

Oxygen-induced defects at the lead halide perovskite/graphene oxide interfaces

Here, graphene oxide or its reduced derivative (GO/RGO) replace metal oxides in perovskite photovoltaics to achieve energy band alignment for minimization of the energy barriers at the film interfaces allowing efficient charge transport, and eliminate stability issues. However, the power conversion efficiencies fall in a wide range (~0.6–18%). Therefore, the perovskite growth and nucleation on GO/RGO require fundamental understanding to improve device function for controlled fabrication, which remain a major challenge. We analyze the surface morphology and crystallization of the lead halide perovskites (MAPbX 3 ) at 20–300 °C on GO using X-ray diffraction and photoelectron spectroscopy. To determine defect mechanisms and their composition, we perform in situ transmission infrared and micro Raman spectroscopy, and the cross-sectional scanning microscopy that captures interfacial imperfections with the oxygen defects. We demonstrate the oxygen-induced defects at the MAPbX 3 /GO interfaces that initiate at room temperature, and occur through the nucleophilic substitution reactions. Unexpectedly, structural defects nucleate in GO forming chemically reduced GO, and modify the surface morphology that yield a poor perovskite growth. Our theoretical studies also reveal that energetically favorable, exothermic reactions between the halides of the perovskite precursors and the oxygen groups of GO generate acidic reaction by-products ( i.e. HX), that confirm the formation of oxygen-induced defects.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Inelastic electron tunneling spectroscopy of local “spin accumulation” devices

We investigate the origin of purported “spin accumulation” signals observed in local “three-terminal” (3T) measurements of ferromagnet/insulator/n-Si tunnel junctions using inelastic electron tunneling spectroscopy (IETS). Voltage bias and magnetic field dependences of the IET spectra were found to account for the dominant contribution to 3T magnetoresistance, thus indicating that it arises from inelastic tunneling through impurities and defects at junction interfaces and within the barrier, rather than from spin accumulation due to pure elastic tunneling into bulk Si as has been previously assumed.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗

Capillary barriers for staged loading of microfluidic devices

Various aspects of the present disclosure are directed toward methods and apparatuses for interacting a first liquid and a second liquid in one or more fluidic channels of a capillary structure. The methods and apparatuses can include providing at least one capillary barrier that positions a meniscus of the first liquid at a fluid-interface region using capillary forces within the capillary structure. Additionally, a path is provided along one of the channels for the second liquid to flow toward the fluid-interface region. Additionally, gas pressure is released, via a gas-outflow port, from the fluid-interface region while flow of the first liquid is arrested. Further, the first liquid and the second liquid contact in the fluid-interface region with the capillary barrier holding the first liquid at the fluid-interface region.

Santiago, Juan G.↗

Integrating atomic layer deposition and ultra-high vacuum physical vapor deposition for in situ fabrication of tunnel junctions

Atomic Layer Deposition (ALD) is a promising technique for growing ultrathin, pristine dielectrics on metal substrates, which is essential to many electronic devices. Tunnel junctions are an excellent example which require a leak-free, ultrathin dielectric tunnel barrier of typical thickness around 1 nm between two metal electrodes. A challenge in the development of ultrathin dielectric tunnel barriers using ALD is controlling the nucleation of dielectrics on metals with minimal formation of native oxides at the metal surface for high-quality interfaces between the tunnel barrier and metal electrodes. This poses a critical need for integrating ALD with ultra-high vacuum (UHV) physical vapor deposition. In order to address these challenges, a viscous-flow ALD chamber was designed and interfaced to an UHV magnetron sputtering chamber via a load lock. A sample transportation system was implemented for in situ sample transfer between the ALD, load lock, and sputtering chambers. Using this integrated ALD-UHV sputtering system, superconductor-insulator-superconductor (SIS) Nb-Al/Al{sub 2}O{sub 2}/Nb Josephson tunnel junctions were fabricated with tunnel barriers of thickness varied from sub-nm to ∼1 nm. The suitability of using an Al wetting layer for initiation of the ALD Al{sub 2}O{sub 3} tunnel barrier was investigated with ellipsometry, atomic force microscopy, and electrical transport measurements. With optimized processing conditions, leak-free SIS tunnel junctions were obtained, demonstrating the viability of this integrated ALD-UHV sputtering system for the fabrication of tunnel junctions and devices comprised of metal-dielectric-metal multilayers.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗

Analysis of interfaces in Bornite (Cu5FeS4) fabricated Schottky diode using impedance spectroscopy method and its photosensitive behavior

Highlights: • Impedance spectroscopy study and current-voltage analysis of Bornite fabricated Schottky diode. • Analysis of interface regions of Schottky barrier diode under dc bias voltage. • Deduction of photosensing parameters for Al/Cu{sub 5}FeS{sub 4}/FTO Schottky diode. • Discussion of charge transport mechanism by employing space charge limited current (SCLC) theory. - Abstract: In this report, we have synthesized Bornite (Cu{sub 5}FeS{sub 4}) material by hydrothermal synthesis technique. The interface characteristics of Al/Cu{sub 5}FeS{sub 4}/FTO Schottky barrier diode (SBD) are investigated by using ac impedance spectroscopy (IS) analysis (under dark condition) and dc current-voltage (I–V) measurements (under dark and light both condition). IS is a powerful tool to identify the interface regions of SBDs. Ac impedance spectra of Al/Cu{sub 5}FeS{sub 4} SBD are recorded in the frequency range 40 Hz-20 MHz during dc bias scanning from -0.6 V to 0.6 V under dark condition. The diode parameter including ideality factor and barrier height is calculated from the conventional I–V measurement based on thermionic emission (TE) theory. Space charge limited current (SCLC) theory has been employed to further exemplify the improved performance of Cu{sub 5}FeS{sub 4} based SBD, which points out that the carrier mobility is enhanced ∼2-fold after irradiation of light.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗

Reactions at noble metal contacts with methylammonium lead triiodide perovskites: Role of underpotential deposition and electrochemistry

Chemical reactivity of halide perovskites coupled with a low energy of formation makes it a challenge to characterize material properties and achieve long-term device stability. In this study, we elucidate electrochemical reactions occurring at the methylammonium lead triiodide (MAPbI 3 )/Au interface. X-ray photoemission spectroscopy is used to identify a type of reduction/oxidation reaction termed underpotential deposition (UPD) involving lead, iodine, and hydrogen occurring at interfaces with noble metals. Changes in surface compositions and oxidation states suggest that UPD derived adsorbates at MAPbI 3 /Au interfaces lower the energy barrier for release of volatile HI and/or I 2 catalyzing degradation at exposed contacts. Additionally, comparison to PbI 2 /Au interfaces demonstrates that the presence of methylammonium/methylamine accelerates the formation of a Pb 0 adlayer on the Au. Reactions involving UPD Pb 0 can transform the typically anodic (hole collecting) Au to a cathode in a photovoltaic measurement. Cyclic voltammetry reveals electrochemical reaction peaks in indium tin oxide (ITO)/MAPbI 3 /Au devices occurring within voltage ranges commonly used for perovskite characterization. The electrochemical stability window of this device architecture is measured to be between -0.5 V and 0.9 V. Voltage induced interfacial reactions contribute to reversible electrochemical peaks, hysteresis, switchable perovskite diode polarity, and permanent degradation at larger voltages. These types of surface reactions alter the interface/interphase composition beyond ion accumulation, provide a source for the diffusion of defects, and contribute to electrode material dependent current-voltage hysteresis. Moreover, the results imply fundamental limitations to achieving high device stability with noble metals and/or methylammonium containing perovskites.

36 MATERIALS SCIENCE↗

Interface scattering in polycrystalline thermoelectrics

We study the effect of electron and phonon interface scattering on the thermoelectric properties of disordered, polycrystalline materials (with grain sizes larger than electron and phonons' mean free path). Interface scattering of electrons is treated with a Landauer approach, while that of phonons is treated with the diffuse mismatch model. The interface scattering is embedded within a diffusive model of bulk transport, and we show that, for randomly arranged interfaces, the overall system is well described by effective medium theory. Using bulk parameters similar to those of PbTe and a square barrier potential for the interface electron scattering, we identify the interface scattering parameters for which the figure of merit ZT is increased. We find the electronic scattering is generally detrimental due to a reduction in electrical conductivity; however, for sufficiently weak electronic interface scattering, ZT is enhanced due to phonon interface scattering.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗

Insulating-layer formation of metallic LaNiO{sub 3} on Nb-doped SrTiO{sub 3} substrate

We investigated the electronic structures of strongly correlated metallic LaNiO{sub 3} (LNO) and semiconducting Nb-doped SrTiO{sub 3} (Nb:STO) heterostructures by varying the LNO film thickness using in situ photoemission spectroscopy. We found that, contrary to other interfaces with SrTiO{sub 3} and LaAlO{sub 3}, insulating LNO layers are formed between metallic LNO layers and Nb:STO. Such behavior seems to be related with an electron transfer from Nb:STO to LNO due to Schottky-barrier formation at the interface.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗

Diamine chelates for increased stability in mixed Sn–Pb and all-perovskite tandem solar cells

Perovskite tandem solar cells show promising performance but non-radiative recombination and its progressive worsening with time, especially in the mixed Sn–Pb low-bandgap layer, limit performance and stability. Here, in this study, we find that mixed Sn–Pb perovskite thin films exhibit a compositional gradient, with an excess of Sn on the surface – and we show this gradient exacerbates oxidation and increases the recombination rate. We find that diamines preferentially chelate Sn atoms, removing them from the film surface and achieving a more balanced Sn:Pb stoichiometry, making the surface of the film resistive to the oxidation of Sn. The process forms an electrically resistive low-dimensional barrier layer, passivating defects and reducing interface recombination. Further improving the homogeneity of the barrier layer using 1,2-diaminopropane results in more uniform distribution and passivation. Tandems achieve a power conversion efficiency of 28.8%. As a result, encapsulated tandems retain 90% of initial efficiency following 1000 hours of operating at the maximum power point under simulated one-sun illumination in air without cooling.

14 SOLAR ENERGY↗

Defects‐Induced In‐Plane Heterophase in Cobalt Oxide Nanosheets for Oxygen Evolution Reaction

Abstract Cobalt oxides as efficient oxygen evolution reaction (OER) electrocatalysts have received much attention because of their rich reserves and cheap cost. There are two common cobalt oxides, Co 3 O 4 (spinel phase, stable but poor intrinsic activity) and CoO (rocksalt phase, active but easily be oxidatized). Constructing Co 3 O 4 /CoO heterophase can inherit both characteristic features of each component and form a heterophase interface facilitating charge transfer, which is believed to be an effective strategy in designing excellent electrocatalysts. Herein, an atomic arrangement engineering strategy is applied to improve electrocatalytic activity of Co 3 O 4 for the OER. With the presence of oxygen vacancies, cobalt atoms at tetrahedral sites in Co 3 O 4 can more easily diffuse into interstitial octahedral sites to form CoO phase structure as revealed by periodic density functional theory computations. The Co 3 O 4 /CoO spinel/rocksalt heterophase can be in situ fabricated at the atomic scale in plane. The overpotential to reach 10 mA cm −2 of Co 3 O 4 /CoO is 1.532 V, which is 92 mV smaller than that of Co 3 O 4 . Theoretical calculations confirm that the excellent electrochemical activity is corresponding to a decline in average p ‐state energy of adsorbed‐O on the Co 3 O 4 /CoO heterophase interface. The reaction Gibbs energy barrier has been significantly decreased with the construction of the heterophase interface.

Liu, Zhijuan↗

Study of the oxygen transport through Ag (110), Ag (poly), and Ag 2.0 Zr

The transport of oxygen through high-purity membranes of Ag (110), Ag (poly), Ag (nano), and Ag 2.0 Zr has been studied by an ultrahigh vacuum permeation method over the temperature range of 400-800 C. The data show that there are substantial deviations from ordinary diffusion-controlled transport. A surface limitation has been confirmed by glow-discharge studies where the upstream O2 supply has been partially converted to atoms, which, for the same temperature and pressure, gave rise to over an order of magnitude increase in transport flux. Further, the addition of 2.0 wt percent Zr to the Ag has provided increased dissociative adsorption rates, which, in turn, increased the transport flux by a factor of 2. It was also observed that below a temperature of 630 C, the diffusivity exhibits an increase in activation energy of over 4 kcal/mol, which has been attributed to trapping of the atomic oxygen and/or kinetic barriers at the surface and subsurface of the vacuum interface. Above 630 C, the activation barrier decreases to the accepted value of about 11 kcal/mol for Ag (poly), consistent with zero concentration at the vacuum interface.

Outlaw, R. A.↗

Characterizing the Geometry and Quantifying the Impact of Nanoscopic Electrocatalyst/Semiconductor Interfaces under Solar Water Splitting Conditions

The materials that are receiving the most attention in photoelectrochemical water splitting are metallic nanoparticle electrocatalysts (np-EC) attached to the surface of a semiconductor (SC) light absorber. In these multicomponent systems, the interface between the semiconductor and electrocatalysts critically affects performance. However, the np-EC/SC interface remains poorly understood as it is complex on atomic scales, dynamic under reaction conditions, and inaccessible to direct experimental probes. This contribution sheds light on how the electrocatalyst/semiconductor interface evolves under reaction conditions by investigating the behavior of nickel electrocatalysts (as nanoparticles and films) deposited on silicon semiconductors. Rigorous electrochemical experiments, interfacial atomistic characterization, and computational modeling are combined to demonstrate critical links between the atomistic features of the interface and the overall performance. It is shown that electrolyte-induced atomistic changes to the interface lead to (1) modulation of the charge carrier fluxes and a dramatic decrease in the electron/hole recombination rates and (2) a change in the barrier height of the interface. Additionally, the critical roles of nonidealities and electrocatalyst coverage due to interfacial geometry are explored. Each of these factors must be considered to optimize the design of metal/semiconductor interfaces which are broadly applicable to photoelectrocatalysis and photovoltaic research.

36 MATERIALS SCIENCE↗

Fe-saponite growth on low-carbon and stainless steel in hydrothermal-bentonite experiments

Hydrothermal experiments on engineered barrier system (EBS) materials were conducted to characterize high temperature interactions between bentonite and candidate waste container steels (304SS, 316SS, low-C steel) for deep geological disposition of nuclear spent fuel. In this study, hydrothermal experiments were performed using Dickson reaction cells at temperatures and pressure of up to 300 °C and 15–16 MPa, respectively, for four to six weeks. Wyoming bentonite was saturated with a 1900 ppm K-Ca-Na-Cl solution in combination with stainless and low-C steel coupons. Authigenic Fe-saponite precipitated utilizing steel as a growth substrate with Fe being supplied by steel corrosion. Concurrent with Fe-saponite formation, sulfides precipitated from sulfide-bearing fluids, from pyrite dissolution, near the steel interface. Sulfide mineral formation is dependent on the steel substrate composition: stainless steel produced pentlandite ((Ni, Fe) 9 S 8 ) and millerite (NiS), whereas low C steel generated pyrrhotite (Fe 7 S 8 ). The presence of sulfides suggests highly reduced environments at the steel-clay barrier interface potentially influencing overall steel corrosion rates and (re)passivation mechanisms. Finally, results of this research show that nuclear waste steel container material may act as a substrate for mineral growth in response to corrosion during hydrothermal interactions with bentonite barriers.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗