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Nb-doped SnO 2 (NTO) thin films were synthesized by atomic layer deposition technique at low temperature (100 °C). For an efficient incorporation of the Nb atoms, i.e. fine control of their amount and distribution, various supercycle ratios and precursor pulse sequences were explored. The thin film growth process studied by in-situ QCM revealed that the Nb incorporation is highly impacted by the surface nature as well as the amount of species available at the surface. This was confirmed by the actual concentration of the Nb atom incorporated inside the thin film as determined by XPS. Highly transparent thin films which transmit more than 95% of the AM1.5 global solar irradiance over a wide spectral range (300-1000 nm) were obtained. In addition, the Nb atoms influenced the optical band gap, conduction band, and valence band levels. While SnO 2 thin film were too resistive, films tuned to conductive nature upon Nb incorporation with controlled concentration. Optimal incorporation level was found to be ⩽1 at.% of Nb, and carrier concentration reached up 2.5 × 10 18 cm -3 for the as-deposited thin films. As a result, the high optical transparency accompanied with tuned electrical property of NTO thin films fabricated by ALD at low temperature paves the way for their integration into temperature-sensitive, nanostructured optoelectrical devices., (© 2024 IOP Publishing Ltd.)

Perovskite solar cells (PSCs) offer impressive performance and flexibility, thanks to their simple, low-temperature deposition methods. Their band gap tunability allows for a wide range of applications, transitioning from opaque to transparent devices. This study introduces the first flexible, bifacial PSCs using the FAPbBr 3 perovskite. We investigated the impact of optimizing electron and hole transport layers on the cells' bifaciality, transparency, and stability. PSCs achieved a maximum power conversion efficiency (PCE) of 6.8 and 18.7% under 1 sun and indoor light conditions (1200 lx), respectively, showing up to 98% bifaciality factor and an average visible transmittance (AVT) of 55%. Additionally, a P1-P2-P3 laser ablation scheme has been developed on the flexible poly(ethylene terephthalate) (PET) substrate for perovskite solar modules showing a PCE of 4.8% and high geometrical fill factor (97.8%). These findings highlight the potential of flexible, bifacial PSCs for diverse applications such as building-integrated photovoltaics (BIPV), agrivoltaics, automotive technology, wearable sensors, and Internet of things (IoT).

Memristor-based neural networks provide an exceptional energy-efficient platform for artificial intelligence (AI), presenting the possibility of self-powered operation when paired with energy harvesters. However, most memristor-based networks rely on analog in-memory computing, necessitating a stable and precise power supply, which is incompatible with the inherently unstable and unreliable energy harvesters. In this work, we fabricated a robust binarized neural network comprising 32,768 memristors, powered by a miniature wide-bandgap solar cell optimized for edge applications. Our circuit employs a resilient digital near-memory computing approach, featuring complementarily programmed memristors and logic-in-sense-amplifier. This design eliminates the need for compensation or calibration, operating effectively under diverse conditions. Under high illumination, the circuit achieves inference performance comparable to that of a lab bench power supply. In low illumination scenarios, it remains functional with slightly reduced accuracy, seamlessly transitioning to an approximate computing mode. Through image classification neural network simulations, we demonstrate that misclassified images under low illumination are primarily difficult-to-classify cases. Our approach lays the groundwork for self-powered AI and the creation of intelligent sensors for various applications in health, safety, and environment monitoring., (© 2024. The Author(s).)

Research on metal halide perovskites as absorbers for X-ray detection is an attractive subject due to the optimal optoelectronic properties of these materials for high-sensitivity applications. However, the contact degradation and the long-term instability of the current limit the performance of the devices, in close causality with the dual electronic-ionic conductivity of these perovskites. Herein, millimeter-thick methylammonium-lead bromide (MAPbBr 3 ) single and polycrystalline samples are approached by characterizing their long-term dark current and photocurrent under X-ray incidence. It is shown how both the dark current and the sensitivity of the detectors follow similar trends at short-circuit ( V = 0 V) after biasing. By performing drift-diffusion numerical simulations, it is revealed how large ionic-related built-in fields not only produce relaxations to equilibrium lasting up to tens of hours but also continue to affect the charge kinetics under homogeneous low photogeneration rates. Furthermore, a method is suggested for estimating the ionic mobility and concentration by analyzing the initial current at short-circuit and the characteristic diffusion times., Competing Interests: The authors declare no competing financial interest., (© 2023 The Authors. Published by American Chemical Society.)

The evolution of ferroelectric instability in ABO 3 perovskites is systematically investigated for tantalates, niobates and titanates at the hybrid density-functional theory level. The influence of the A cation is analysed in terms of the frequency of the lowest F 1u IR-active phonon mode at different volumes for (Cs, Rb, K, Na)TaO 3 , (Ba, Pb, Sn, Ge)TiO 3 and (Rb, K, Na, Li)NbO 3 and correlated with the ionic radius as well as the degree of hybridization in the bonds. The atomic displacement corresponding to each mode is described as a function of volume, and the static permittivity is calculated for the stable Pm 3̄ m phases. It is shown that the amplitude of the atomic displacements associated with the soft mode linked to the ferroelectric instability increases at a given volume when the ionic radius of the cation A decreases and when the hybridization of the B-O bond increases. This provides criteria for optimizing the dielectric properties of materials and for suggesting effective solid solutions. Tantalum perovskites presenting para-ferroelectric phase transitions, some of which are close to ambient conditions, are interesting materials for high-permittivity dielectrics in view of lead-free compounds with a high static dielectric response.

With their unique structural, optical and electrical properties, III-V nanowires (NWs) are an extremely attractive option for the direct growth of III-Vs on Si for tandem solar cell applications. Here, we introduce a core-shell GaAs/GaInP NW solar cell grown by molecular beam epitaxy on a patterned Si substrate, and we present an in-depth investigation of its optoelectronic properties and limitations. We report a power conversion efficiency of almost 3.7%, and a state-of-the-art open-circuit voltage ( V OC ) for a NW array solar cell on Si of 0.65 V. We also present the first quantification of the quasi-Fermi level splitting in NW array solar cells using hyperspectral photoluminescence measurements. A value of 0.84 eV is obtained at 1 sun (1.01 eV at 81 suns), which is significantly higher than q V OC . It indicates NWs with a better intrinsic optoelectronic quality than what could be expected from TEM images or deduced from electrical measurements. Optical and electronic simulations provide insights into the main absorption and electrical losses, and guidelines to design and fabricate higher-efficiency devices. It suggests that improvements at the n-type contact (GaInP/ITO) are key to unlocking the potential of next generation NW solar cells.

We describe the investigation of metal halide perovskite layers, particularly CH 3 NH 3 PbI 3 used in photovoltaic applications, by soft X-ray scanning transmission X-ray microscopy (STXM). Relevant reference spectra were used to fit the experimental data using singular value decomposition. The distribution of key elements Pb, I, and O was determined throughout the layer stack of two samples prepared by wet process. One sample was chosen to undergo electrical biasing. Spectral data shows the ability of STXM to provide relevant chemical information for these samples. We found the results to be in good agreement with the sample history, both regarding the deposition sequence and the degradation of the perovskite material., Competing Interests: There are no conflicts to declare., (This journal is © The Royal Society of Chemistry.)

Interface engineering through passivating agents, in the form of organic molecules, is a powerful strategy to enhance the performance of perovskite solar cells. Despite its pivotal function in the development of a rational device optimization, the actual role played by the incorporation of interfacial modifications and the interface physics therein remains poorly understood. Here, we investigate the interface and device physics, quantifying charge recombination and charge losses in state-of-the-art inverted solar cells with power conversion efficiency beyond 23% - among the highest reported so far - by using multidimensional photoluminescence imaging. By doing that we extract physical parameters such as quasi-Fermi level splitting (QFLS) and Urbach energy enabling us to assess that the main passivation mechanism affects the perovskite/PCBM ([6,6]-phenyl-C 61 -butyric acid methyl ester) interface rather than surface defects. In this work, by linking optical, electrical measurements and modelling we highlight the benefits of organic passivation, made in this case by phenylethylammonium (PEAI) based cations, in maximising all the photovoltaic figures of merit., (© 2022. The Author(s).)

Cathodoluminescence mapping is used as a contactless method to probe the electron concentration gradient of Te-doped GaAs nanowires. The room temperature and low temperature (10 K) cathodoluminescence analysis method previously developed for GaAs:Si is first validated on five GaAs:Te thin film samples, before extending it to the two GaAs:Te NW samples. We evidence an electron concentration gradient ranging from below 1 × 10 18 cm -3 to 3.3 ×10 18 cm -3 along the axis of a GaAs:Te nanowire grown at 640 °C, and a homogeneous electron concentration of around 6-8 × 10 17 cm -3 along the axis of a GaAs:Te nanowire grown at 620 °C. The differences in the electron concentration levels and gradients between the two nanowires is attributed to different Te incorporation efficiencies by vapor-solid and vapor-liquid-solid processes., (© 2022 IOP Publishing Ltd.)

Noble metal coordination xerogel films (mesostructured with block-copolymers) exhibit solubility switching with increasing X-ray irradiation. Different from other sol-gel systems, these are attributed to film deconstruction under irradiation. These materials can be used as recyclable negative tone resists for deep X-ray lithography that can be further converted into metallic nanoarchitectured films.

Noble metal nanostructured films are of great interest for various applications including electronics, photonics, catalysis, and photocatalysis. Yet, structuring and patterning noble metals, especially those of the platinum group, is challenging by conventional nanofabrication. Herein, an approach based on solution processing to obtain metal-based films (rhodium, ruthenium (Ru) or iridium in the presence of residual organic species) with nanostructuration at the 20 nm-scale is introduced. Compared to existing approaches, the dual functionality of block-copolymers acting both as structuring and as reducing agent under inert atmosphere is exploited. A set of in situ techniques has allowed for the capturing of the carbothermal reduction mechanism occurring at the hybrid organic/inorganic interface. Differently from previous literature, a two-step reduction mechanism is unveiled with the formation of a carbonyl intermediate. From a technological point of view, the materials can be solution-processed on a large scale by dip-coating as polymers and simultaneously structured and reduced into metals without requiring expensive equipment or treatments in reducing atmosphere. Importantly, the metal-based films can be patterned directly by block-copolymer lithography or by soft-nanoimprint lithography on various substrates. As proof-of-concept of application, the authors demonstrate that nanostructured Ru films can be used as efficient catalysts for H 2 generation into microfluidic reactors., (© 2021 Wiley-VCH GmbH.)

In this article, STEM-EELS methodology is described to investigate the composition of sensitive crystalline Silicon/amorphous aluminum oxide (c-Si/a-AlOx) interface of an a AlOx/amorphous hydrogenated silicon nitride (a-AlOx/a-SiNx:H) passivation stack of a c-Si solar cell. In this stack, a-AlOx has the distinctive characteristic to provide both chemical and field effect passivation, which need further research to be more controlled in order to improve solar cell efficiency. a-AlOx is known to be unstable under the electron-beam, so we first present a detailed study on the electron-beam radiation damage to c-Si/a-AlOx interface. This interface can indeed undergo several electron-beam irradiation damage like sputtering, knock-on or radiolysis if precautions are not taken. Radiolysis damage has been found to be the dominant radiation damage. Thus, several STEM-EELS acquisition parameters like acceleration voltage, electron dose and scan orientation were taken into account and modified to limit this radiolysis damage. Once the irradiation was limited, STEM-EELS investigation was conduct using DualEELS on the Si and Al L2,3 and OK edge fines structures. The interface was found to be composed of a-SiOx and non-stoichiometric aluminum silicate with a predominance of tetrahedrally coordinated Al in its first layer., (Copyright © 2021 Elsevier Ltd. All rights reserved.)

Reaction mechanisms during the growth of multinary compounds by atomic layer deposition can be complex, especially for sulfide materials. For instance, the deposition of copper indium disulfide (CuInS 2 ) shows a non-direct correlation between the cycle ratio, the growth per cycle of each binary growth cycles, i.e., Cu x S and In 2 S 3 , and the film composition. This evidences side reactions that compete with the direct Atomic Layer Deposition (ALD) growth reactions and makes the deposition of large films very challenging. To develop a robust upscalable recipe, it is essential to understand the chemical surface reactions. In this study, reaction mechanisms in the Cu-In-S ternary system were investigated in-situ by using a quartz crystal microbalance system to monitor mass variations. Pure binary indium sulfide (In 2 S 3 ) and copper sulfide (Cu x S) thin film depositions on Al 2 O 3 substrate were first studied. Then, precursors were transported to react on Cu x S and In 2 S 3 substrates. In this paper, gas-phase ion exchanges are discussed based on the recorded mass variations. A cation exchange between the copper precursor and the In 2 S 3 is highlighted, and a solution to reduce it by controlling the thickness deposited for each stack of binary materials during the CuInS 2 deposition is finally proposed., Competing Interests: The authors declare no conflict of interest. The funders had no role in the design of the study; in the collection, analyses, or interpretation of data; in the writing of the manuscript, or in the decision to publish the results.

This work focuses on the extraction of the open circuit voltage (V OC ) on photovoltaic nanowires by surface photovoltage (SPV) based on Kelvin probe force microscopy (KPFM) measurements. In a first approach, P-I-N radial junction (RJ) silicon nanowire (SiNW) devices were investigated under illumination by KPFM and current-voltage (I-V) analysis. Within 5%, the extracted SPV correlates well with the V OC . In a second approach, local SPV measurements were applied on single isolated radial junction SiNWs pointing out shadowing effects from the AFM tip that can strongly impact the SPV assessment. Several strategies in terms of AFM tip shape and illumination orientation have been put in place to minimize this effect. Local SPV measurements on isolated radial junction SiNWs increase logarithmically with the illumination power and demonstrate a linear behavior with the V OC . The results show notably that contactless measurements of the V OC become feasible at the scale of single photovoltaic SiNW devices.

We investigate low-temperature (<200 °C) plasma-enhanced chemical vapor deposition (PECVD) for the formation of p-n junctions. Compared to the standard diffusion or implantation processes, silicon growth at low temperature by PECVD ensures a lower thermal budget and a better control of the doping profile. We previously demonstrated the successful growth of boron-doped epitaxial silicon layers (p+ epi-Si) at 180 °C. In this paper, we study the activation of boron during annealing via dark conductivity measurements of p+ epi-Si layers grown on silicon-on-insulator (SOI) substrates. Secondary Ion Mass Spectroscopy (SIMS) profiles of the samples, carried out to analyze the elemental composition of the p+ epi-Si layers, showed a high concentration of impurities. Finally, we have characterized the p+ epi-Si layers by low-temperature photoluminescence (PL). Results revealed the presence of a broad defect band around 0.9 eV. In addition, we observed an evolution of the PL spectrum of the sample annealed at 200 °C, suggesting that additional defects might appear upon annealing.

We show that mechanochemically synthesized halide perovskite powders from a ball milling approach can be employed to fabricate a variety of lead halide perovskites with exceptional intrinsic stability. Our MAPbI 3 powder exhibits higher thermal stability than conventionally processed thin films, without degradation after more than two and a half years of storage and only negligible degradation after heat treatment at 220 °C for 14 h. We further show facile recovery strategies of nonphase-pure powders by simple remilling or mild heat treatment. Moreover, we demonstrate the mechanochemical synthesis of phase-pure mixed perovskite powders, such as (Cs 0.05 FA 0.95 PbI 3 ) 0.85 (MAPbBr 3 ) 0.15 , from either the individual metal and organic halides or from readily prepared ternary perovskites, regardless of the precursor phase purity. Adding potassium iodide (KI) to the milling process successfully passivated the powders. We also succeeded in preparing a precursor solution on the basis of the powders and obtained uniform thin films for integration into efficient perovskite solar cells from spin-coating this solution. We find the KI passivation remains in the devices, leading to improved performance and significantly reduced hysteresis. Our work thus demonstrates the potential of mechanochemically synthesized halide perovskite powders for long-time storage and upscaling, further paving the way toward commercialization of perovskite-based optoelectronic devices.

We present an effective method of determining the doping level in n-type III-V semiconductors at the nanoscale. Low-temperature and room-temperature cathodoluminescence (CL) measurements are carried out on single Si-doped GaAs nanowires. The spectral shift to higher energy (Burstein-Moss shift) and the broadening of luminescence spectra are signatures of increased electron densities. They are compared to the CL spectra of calibrated Si-doped GaAs layers, whose doping levels are determined by Hall measurements. We apply the generalized Planck's law to fit the whole spectra, taking into account the electron occupation in the conduction band, the bandgap narrowing, and band tails. The electron Fermi levels are used to determine the free electron concentrations, and we infer nanowire doping of 6 × 10 17 to 1 × 10 18  cm -3 . These results show that cathodoluminescence provides a robust way to probe carrier concentrations in semiconductors with the possibility of mapping spatial inhomogeneities at the nanoscale.

Alzheimer's disease is a challenge of the utmost importance for contemporary society. An early diagnosis is essential for the development of treatments and for establishing a network of support for the patient. In this light, the deposition in the brain of amyloid-β fibrillar aggregates, which is a distinctive feature of Alzheimer, is key for an early detection of this disease. In this work we propose an atomistic study of the interaction of amyloid tracers with recently published polymorphic models of amyloid-β 1-40 and 1-42 fibrils, highlighting the relationship between marker architectures and binding affinity. This work uncovers the importance of quaternary structure, and in particular of junctions between amyloid-β protofilaments, as the key areas for marker binding.

The search for functional materials is currently hindered by the difficulty to find significant correlation between constitutive properties of a material and its functional properties. In the case of amorphous materials, the diversity of local structures, chemical composition, impurities and mass densities makes such a connection difficult to be addressed. In this Letter, the relation between refractive index and composition has been investigated for amorphous AlO x materials, including nonstoichiometric AlO x , emphasizing the role of structural defects and the absence of effect of the band gap variation. It is found that the Newton-Drude (ND) relation predicts the refractive index from mass density with a rather high level of precision apart from some structures displaying structural defects. Our results show especially that O- and Al-based defects act as additive local disturbance in the vicinity of band gap, allowing us to decouple the mass density effects from defect effects (n = n[ND] + Δn defect ).

The substitution of lithium for copper in Cu 2 ZnSnS 4 (CZTS) has been experimentally and theoretically investigated. Formally, the (Cu 1-x Li x )ZnSnS 4 system exhibits two well-defined solid solutions. Indeed, single crystal structural analyses demonstrate that the low (x < 0.4) and high (x > 0.6) lithium-content compounds adopt the kesterite structure and the wurtz-kesterite structure, respectively. For x between 0.4 and 0.6, the two aforementioned structure types coexist. Moreover, 119 Sn NMR analyses carried out on a (Cu 0.7 Li 0.3 ) 2 ZnSnS 4 sample clearly indicate that lithium replaces copper preferentially on two of the three available 2-fold crystallographic sites commonly occupied by Cu and Zn in disordered kesterite. Furthermore, the observed individual lines in the NMR spectrum suggest that the propensity of Cu and Zn atoms to be randomly distributed over the 2c and 2d crystallographic sites is lowered when lithium is partially substituted for copper. Additionally, the first-principles calculations provide insights into the arrangement of Li atoms as a function of the Cu/Zn disorder and its effect on the structural (lattice parameters) and optical properties of CZTS (band gap evolution). Those calculations agree with the experimental observations and account for the evolutions of the unit cell parameters as well as for the increase of band gap when the Li-content increases. The calculation of the formation enthalpy of point defect unambiguously indicates that Li modifies the Cu/Zn disorder in a manner similar to the change of Cu/Zn disorder induced by Ag alloying. Overall, it was found that Li alloying is a versatile way of tuning the optoelectronic properties of CZTS making it a good candidate as wide band gap materials for the top cells of tandem solar cells.