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At least 631 records · Page 35

Reduced recombination via tunable surface fields in perovskite thin films

Here, the ability to reduce energy loss at semiconductor surfaces through passivation or surface field engineering is an essential step in the manufacturing of efficient photovoltaic (PV) and optoelectronic devices. Similarly, surface modification of emerging halide perovskites with quasi-two-dimensional (2D) heterostructures is now ubiquitous to achieve PV power conversion efficiencies (PCEs) >25%, yet a fundamental understanding to how these treatments function is still generally lacking. Here we use a unique combination of depth-sensitive nanoscale characterization techniques to uncover a tunable passivation strategy and mechanism found in perovskite PV devices that were the first to reach the >25% PCE milestone. Namely, treatment with hexylammonium bromide leads to the simultaneous formation of an iodide-rich 2D layer along with a Br halide gradient that extends from defective surfaces and grain boundaries into the bulk three-dimensional (3D) layer. This interface can be optimized to extend the charge carrier lifetime to record values >30 μs and to reduce interfacial recombination velocities to values as low as <7 cm s −1 .

Devices for energy harvesting↗

Observationally derived rise in methane surface forcing mediated by water vapour trend

Atmospheric methane (CH4) mixing ratios exhibited a plateau between 1995 and 2006 and have subsequently been increasing. While there are a number of competing explanations for the temporal evolution of this greenhouse gas, these prominent features in the temporal trajectory of atmospheric CH4 are expected to perturb the surface energy balance through radiative forcing, largely due to the infrared radiative absorption features of CH4. However, to date this has been determined strictly through radiative transfer calculations. Here, we present a quantified observation of the time series of clear-sky radiative forcing by CH4 at the surface from 2002 to 2012 at a single site derived from spectroscopic measurements along with line-by-line calculations using ancillary data. There was no significant trend in CH4 forcing between 2002 and 2006, but since then, the trend in forcing was 0.026?±?0.006 (99.7%?CI)?W?m2?yr-1. The seasonal-cycle amplitude and secular trends in observed forcing are influenced by a corresponding seasonal cycle and trend in atmospheric CH4. However, we find that we must account for the overlapping absorption effects of atmospheric water vapour (H2O) and CH4 to explain the observations fully. Thus, the determination of CH4 radiative forcing requires accurate observations of both the spatiotemporal distribution of CH4 and the vertically resolved trends in H2O.

Feldman, Daniel R.↗

When are Surface Plasmon Polaritons Excited in the Kretschmann-Raether Configuration?

It is widely believed that the reflection minimum in a Kretschmann-Raether experiment results from direct coupling into surface plasmon polariton modes. Our experimental results provide a surprising discrepancy between the leakage radiation patterns of surface plasmon polaritons (SPPs) launched on a layered gold/germanium film compared to the K-R minimum, clearly challenging this belief. We provide definitive evidence that the reflectance dip in K-R experiments does not correlate with excitation of an SPP mode, but rather corresponds to a particular type of perfectly absorbing (PA) mode. Results from rigorous electrodynamics simulations show that the PA mode can only exist under external driving, whereas the SPP can exist in regions free from direct interaction with the driving field. These simulations show that it is possible to indirectly excite propagating SPPs guided by the reflectance minimum in a K-R experiment, but demonstrate the efficiency can be lower by more than a factor of 3. We find that optimal coupling into the SPP can be guided by the square magnitude of the Fresnel transmission amplitude.

Foley IV, Jonathan J.↗

Electrical bending actuation of gold-films with nanotextured surfaces

An actuating material system comprising a gold-film with nanotextured surface was fabricated. Using electroless gold plating onto a substrate of porous anodized aluminum oxide, a thin film of gold with a high density of short gold nanofibers on its surface was made. When one end of such a film was connected to an ion generator, bending was achieved upon electrical charging in air. Experiments showed that the free end of an 8 mm film could be displaced by more than 1.6 mm with a bending strain of 0.08%. In contrast with other types of thin-film artificial muscle materials, the present Au-film did not require any electrolyte to function. With the relatively easy fabrication method, this nanotextured film shows promising actuation behavior in air. Actuation systems based on a number of mechanisms have been developed in the last few decades, including electric, ionic, photonic, pneumatic, and thermal. As discussed in detail in Madden et al. and Brochu and Pei,11 the weaknesses of these materials include bulkiness, low stress or strain generation, low strain rate, long response time, short cycle life, and low energy efficiency. Recent developments have involved the possibilities to use the unique properties of nanostructures to produce actuation, such as in nanostructured carbon, nanoporous gold or platinum, V 2 O 5 nanofibre sheet, electroactive nanostructured polymers, hybrid carbon nanotube yarn, niobium nanowire yarn, and anodized aluminum oxide (AAO). Here, we introduce a nanostructured material system comprising a gold film with a high density of short gold-nanofibers attached to one side, which can bend to produce a large displacement (~1.6 mm) upon electrical charging through an ion generator. In addition to the displacement, the functionality without the need of an electrolyte is another advantage for using this material system as actuators. We discuss the fabrication and characterization methods, the morphology, and the actuating properties of this system here. To achieve a metal film with a nanotextured surface, electroless gold-plating was performed on substrates of AAO with a characteristic nano-honeycomb structure consisting of >10 10 pores per cm 2 . The fabrication of the AAO substrates followed the procedures described in Cheng and Ngan. The anodization condition for the AAO was 40 V against graphite electrode in saturated oxalic acid at 18 °C for 2 h. The pore diameter observed was 50 ± 5 nm. By using an electroless gold-plating method described by Kohli et al.,22 gold in short nanofiber form was deposited into the pores of the AAO template. As shown in Figs. 1(a) and 1(b), in addition to partially filling the pores with gold, the top surface of the AAO template was coated with a thin gold film (~100 nm) of Au. A ~30 μm layer of lacquer was then painted on the top of the thin gold film to serve as a supporting layer.

42 ENGINEERING↗

A dual wavelength imaging system for plasma-surface interaction studies on the National Spherical Torus Experiment Upgrade

A two-channel spectral imaging system based on a charge injection device radiation-hardened intensified camera was built for studies of plasma-surface interactions on divertor plasma facing components in the National Spherical Torus Experiment Upgrade (NSTX-U) tokamak. By means of commercially available mechanically referenced optical components, the two-wavelength setup images the light from the plasma, relayed by a fiber optic bundle, at two different wavelengths side-by-side on the same detector. Remotely controlled filter wheels are used for narrow bandpass and neutral density filters on each optical path allowing for simultaneous imaging of emission at wavelengths differing in brightness up to 3 orders of magnitude. Applications on NSTX-U will include the measurement of impurity influxes in the lower divertor strike point region and the imaging of plasma-material interaction on the head of the surface analysis probe MAPP (Material Analysis and Particle Probe). The diagnostic setup and initial results from its application on the lithium tokamak experiment are presented.

46 INSTRUMENTATION RELATED TO NUCLEAR SCIENCE AND ↗

Ligand-surface interactions and surface oxidation of colloidal PbSe quantum dots revealed by thin-film positron annihilation methods

Positron Two Dimensional Angular Correlation of Annihilation Radiation (2D-ACAR) measurements reveal modifications of the electronic structure and composition at the surfaces of PbSe quantum dots (QDs), deposited as thin films, produced by various ligands containing either oxygen or nitrogen atoms. In particular, the 2D-ACAR measurements on thin films of colloidal PbSe QDs capped with oleic acid ligands yield an increased intensity in the electron momentum density (EMD) at high momenta compared to PbSe quantum dots capped with oleylamine. Moreover, the EMD of PbSe QDs is strongly affected by the small ethylenediamine ligands, since these molecules lead to small distances between QDs and favor neck formation between near neighbor QDs, inducing electronic coupling between neighboring QDs. The high sensitivity to the presence of oxygen atoms at the surface can be also exploited to monitor the surface oxidation of PbSe QDs upon exposure to air. Finally, our study clearly demonstrates that positron annihilation spectroscopy applied to thin films can probe surface transformations of colloidal semiconductor QDs embedded in functional layers.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Controlling the surface photovoltage on WSe 2 by surface chemical modification

The surface photovoltage (SPV) effect is key to the development of opto-electronic devices such as solar-cells and photo-detectors. For the prototypical transition metal dichalcogenide WSe 2 , core level and valence band photoemission measurements show that the surface band bending of pristine cleaved surfaces can be readily modified by adsorption with K (an electron donor) or C 60 (an electron acceptor). Time-resolved pump-probe photoemission measurements reveal that the SPV for pristine cleaved surfaces is enhanced by K adsorption, but suppressed by C 60 adsorption, and yet the SPV relaxation time is substantially shortened in both cases. Evidently, adsorbate-induced electronic states act as electron-hole recombination centers that shorten the carrier lifetime.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Parametric Finite Element Analysis of Naturally Corroded Steel Specimens Using 3D Surface Laser Scans

Corrosion is considered a uniform thickness reduction design guideline of the maritime industry. However, additionally, the corroded and irregular morphology of the surface affects the steel's load-bearing capacity and its impact on the strength and elongation behaviour of the steel is not yet fully understood. These effects on the local behaviour of steel structures under tensile loading were investigated with tensile tests on naturally corroded steel specimens and nonlinear finite element simulations including the corroded surface morphology with a uniform surface idealation. The models also include the deformed specimen shape. The developed approach led to highly accurate parametric finite element models predicting the ultimate tensile strength and longitudinal position of fracture. The results show that all included aspects are essential for accurate simulations, while solely the maximum available surface resolution was not as decisive.

corrosion↗

Co-GISAXS technique for investigating surface growth dynamics

Detailed quantitative measurement of surface dynamics during thin film growth is a major experimental challenge. Here X-ray Photon Correlation Spectroscopy with coherent hard X-rays is used in a Grazing-Incidence Small-Angle X-ray Scattering (i.e. Co-GISAXS) geometry as a new tool to investigate nanoscale surface dynamics during sputter deposition of a-Si and a-WSi2 thin films. For both films, kinetic roughening during surface growth reaches a dynamic steady state at late times in which the intensity autocorrelation function g2(q,t) becomes stationary. The g2(q,t) functions exhibit compressed exponential behavior at all wavenumbers studied. The overall dynamics are complex, but the most surface sensitive sections of the structure factor and correlation time exhibit power law behaviors consistent with dynamical scaling.

Rainville, Meliha G.↗

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↗

Surface electron modulation of metal oxide‐based electrochemical devices by surface additives—linking sensors and fuel cells

Abstract The interaction between ambient oxygen and the metal oxide surface is central to various electrochemical devices. Solid oxide fuel cell cathodes and semiconducting metal oxide gas sensors are two prominent examples. Parallels between these two systems are highlighted in this perspective. In both cases, the presence of foreign surface species has been found to significantly alter the interactions of the metal oxides’ surfaces with oxygen. On the one hand, interactions are hindered due to the presence of certain impurities, such as the degradation of fuel cell cathode by Si‐species that originate from processing or from operating environments. On the other hand, electrochemically active noble metal additives have been intentionally used to tune the sensor response of metal oxides. In the case of electrochemically active additives, the need for operando spectroscopies to elucidate the mechanism is discussed. Electronic coupling of the surface additive with the metal oxide is found to play a central role in both cases. We use these results to demonstrate that insights gained from either field can be effectively applied to the other.

Materials Science↗

Reactivity of heterogeneous surfaces: Modeling precursor–surface interaction using absorbing Markov chains

Heterogeneous reactive surfaces involving a spatial distribution of reactive sites are ubiquitous in thin film growth, from defect nucleation to step flow growth. In this work, the interaction of gas phase species with heterogeneous reactive surfaces was explored using a model combining absorbing Markov chains and local balance equations. Through this model, single particle statistics can be extracted of the adsorption-diffusion-desorption/reaction process even beyond the transport-limited regime, where the surface coverage of adsorbates, and hence adsorbate-adsorbate interaction, is not negligible, and local rates can be connected with macroscopic quantities, such as the sticking probability and desorption rates. In the transport-limited regime, a similarity law was identified for the sticking probability for both step flow growth and nucleation on randomly distributed reactive sites in which the sticking probability is a function of the product of the local diffusion and reaction probabilities. Lastly, the model can be applied to extract local reactivity maps providing the probability that a particle adsorbing on a given site reacts with the surface. This allows one to explore the development of capture zones and the impact of site-blocking and desorption on the local sticking probabilities.

36 MATERIALS SCIENCE↗

Supertwisted spirals of layered materials enabled by growth on non-Euclidean surfaces

Using curves to make twists The growth of layered materials on flat substrates usually occurs in stacked layers, although defects or a lattice mismatch can induce strains that distort the shape of subsequent layers. However, these effects are usually small and can be uncontrolled. Zhao et al. now demonstrate the possibility of synthesizing multilayers of two-dimensional materials with certain twists between the layers induced by the presence of screw dislocations in combination with curved substrate surfaces. Different twist angles are achieved by varying the amount of nonplanarity and the character (conical or hyperbolic) of the surface. Science , this issue p. 442

Science & Technology - Other Topics↗