Phase Segregation Mechanisms in Mixed-Halide CsPb(BrI) Nanocrystals in Dependence of Their Sizes and Their Initial [Br]:[I] Ratios.

Phase segregation in inorganic CsPb(BrI) nanoparticles (NPs) exhibiting originally a homogeneous [Br]:[I] mixture was investigated by means of in situ transmission electron microscopy (TEM) and evaluated by using multivariate analyses. The colloidal synthesis of the NPs offers good control of the halide ratios on the nanoscale. The spatially resolved TEM investigations were correlated with integral photoluminescence measurements.

Fast Near-Infrared Photodetectors Based on Nontoxic and Solution-Processable AgBiS.

Solution-processable near-infrared (NIR) photodetectors are urgently needed for a wide range of next-generation electronics, including sensors, optical communications and bioimaging. However, it is rare to find photodetectors with >300 kHz cut-off frequencies, especially in the NIR region, and many of the emerging inorganic materials explored are comprised of toxic elements, such as lead. Herein, solution-processed AgBiS photodetectors with high cut-off frequencies under both white light (>1 MHz) and NIR (approaching 500 kHz) illumination are developed.

Surface-Mediated Charge Transfer of Photogenerated Carriers in Diamond.

Solvated electrons are highly reductive chemical species whose chemical properties remain largely unknown. Diamond materials are proposed as a promising emitter of solvated electrons and visible light excitation would enable solar-driven CO or N reductions reactions in aqueous medium. But sub-bandgap excitation remains challenging.

Managing Excess Lead Iodide with Functionalized Oxo-Graphene Nanosheets for Stable Perovskite Solar Cells.

Stability issues could prevent lead halide perovskite solar cells (PSCs) from commercialization despite it having a comparable power conversion efficiency (PCE) to silicon solar cells. Overcoming drawbacks affecting their long-term stability is gaining incremental importance. Excess lead iodide (PbI ) causes perovskite degradation, although it aids in crystal growth and defect passivation.

Internal electric fields control triplet formation in halide perovskite-sensitized photon upconverters.

Halide perovskite-based photon upconverters utilize perovskite thin films to sensitize triplet exciton formation in a small-molecule layer, driving triplet-triplet annihilation upconversion. Despite having excellent carrier mobility, these systems suffer from inefficient triplet formation at the perovskite/annihilator interface. We studied triplet formation in formamidinium-methylammonium lead iodide/rubrene bilayers using photoluminescence and surface photovoltage methods.

Is Cu P a Semiconductor, a Metal, or a Semimetal?

Despite the recent surge in interest in Cu P for catalysis, batteries, and plasmonics, the electronic nature of Cu P remains unclear. Some studies have shown evidence of semiconducting behavior, whereas others have argued that Cu P is a metallic compound. Here, we attempt to resolve this dilemma on the basis of combinatorial thin-film experiments, electronic structure calculations, and semiclassical Boltzmann transport theory.

Slot-Die Coated Triple-Halide Perovskites for Efficient and Scalable Perovskite/Silicon Tandem Solar Cells.

Wide bandgap halide perovskite materials show promising potential to pair with silicon bottom cells. To date, most efficient wide bandgap perovskites layers are fabricated by spin-coating, which is difficult to scale up. Here, we report on slot-die coating for an efficient, 1.

Accelerating research on novel photovoltaic materials.

The development of new materials typically takes many years or even decades. This has been particularly true for photovoltaic (PV) technologies, which require control of defects on the parts-per-million-level and consist of relatively complex device structures comprising many elements and interfaces between materials. This means that optical and electronic properties can be difficult to pin down, and also heavily depend on the details of processing.

Strong absorption and ultrafast localisation in NaBiS nanocrystals with slow charge-carrier recombination.

I-V-VI ternary chalcogenides are gaining attention as earth-abundant, nontoxic, and air-stable absorbers for photovoltaic applications. However, the semiconductors explored thus far have slowly-rising absorption onsets, and their charge-carrier transport is not well understood yet. Herein, we investigate cation-disordered NaBiS nanocrystals, which have a steep absorption onset, with absorption coefficients reaching >10 cm just above its pseudo-direct bandgap of 1.

Crystallize It before It Diffuses: Kinetic Stabilization of Thin-Film Phosphorus-Rich Semiconductor CuP.

Numerous phosphorus-rich metal phosphides containing both P-P bonds and metal-P bonds are known from the solid-state chemistry literature. A method to grow these materials in thin-film form would be desirable, as thin films are required in many applications and they are an ideal platform for high-throughput studies. In addition, the high density and smooth surfaces achievable in thin films are a significant advantage for characterization of transport and optical properties.

Prediction and realisation of high mobility and degenerate p-type conductivity in CaCuP thin films.

Phosphides are interesting candidates for hole transport materials and p-type transparent conducting applications, capable of achieving greater valence band dispersion than their oxide counterparts due to the higher lying energy and increased size of the P 3p orbital. After computational identification of the indirect-gap semiconductor CaCuP as a promising candidate, we now report reactive sputter deposition of phase-pure p-type CaCuP thin films. Their intrinsic hole concentration and hole mobility exceed 1 × 10 cm and 35 cm V s at room temperature, respectively.

Influence of the Rear Interface on Composition and Photoluminescence Yield of CZTSSe Absorbers: A Case for an AlO Intermediate Layer.

The rear interface of kesterite absorbers with Mo back contact represents one of the possible sources of nonradiative voltage losses (Δ) because of the reported decomposition reactions, an uncontrolled growth of MoSe, or a nonoptimal electrical contact with high recombination. Several intermediate layers (IL), such as MoO, TiN, and ZnO, have been tested to mitigate these issues, and efficiency improvements have been reported. However, the introduction of IL also triggers other effects such as changes in alkali diffusion, altered morphology, and modifications in the absorber composition, all factors that can also influence Δ.

Insights into Nucleation and Growth of Colloidal Quaternary Nanocrystals by Multimodal X-ray Analysis.

Copper chalcogenide nanocrystals find applications in photovoltaic inks, bio labels, and thermoelectric materials. We reveal insights in the nucleation and growth during synthesis of anisotropic CuZnSnS nanocrystals by simultaneously performing in situ X-ray absorption spectroscopy (XAS) and small-angle X-ray scattering (SAXS). Real-time XAFS reveals that upon thiol injection into the reaction flask, a key copper thiolate intermediate species is formed within fractions of seconds, which decomposes further within a narrow temperature and time window to form copper sulfide nanocrystals.

Compositional and Interfacial Engineering Yield High-Performance and Stable p-i-n Perovskite Solar Cells and Mini-Modules.

Through the optimization of the perovskite precursor composition and interfaces to selective contacts, we achieved a p-i-n-type perovskite solar cell (PSC) with a 22.3% power conversion efficiency (PCE). This is a new performance record for a PSC with an absorber bandgap of 1.

Comment on "Resolving spatial and energetic distributions of trap states in metal halide perovskite solar cells".

Ni (Research Articles, 20 March 2020, p. 1352) report bulk trap densities of 10 cm and an increase in interfacial trap densities by one to four orders of magnitude from drive-level capacitance profiling of lead halide perovskites. From electrostatic arguments, we show that the results are not trap densities but are a consequence of the geometrical capacitance and charge injection into the perovskite layer.

BaZrS Chalcogenide Perovskite Thin Films by HS Sulfurization of Oxide Precursors.

The earth-abundant ternary compound BaZrS, which crystallizes in the perovskite-type structure, has come into view as a promising candidate for photovoltaic applications. We present the synthesis and characterization of polycrystalline perovskite-type BaZrS thin films. BaZrO precursor layers were deposited by pulsed laser deposition and sulfurized at various temperatures in an argon-diluted HS atmosphere.

Electronic Structure of the CdS/Cu(In,Ga)Se Interface of KF- and RbF-Treated Samples by Kelvin Probe and Photoelectron Yield Spectroscopy.

Ambient-pressure Kelvin probe and photoelectron yield spectroscopy methods were employed to investigate the impact of the KF and RbF postdeposition treatments (KF-PDT, RbF-PDT) on the electronic features of Cu(In,Ga)Se (CIGSe) thin films and the CdS/CIGSe interface in a CdS thickness series that has been sequentially prepared during the chemical bath deposition (CBD) process depending on the deposition time. We observe distinct features correlated to the CBD-CdS growth stages. In particular, we find that after an initial CBD etching stage, the valence band maximum (VBM) of the CIGSe surface is significantly shifted (by 180-620 mV) toward the Fermi level.

Monolithic perovskite/silicon tandem solar cell with >29% efficiency by enhanced hole extraction.

Tandem solar cells that pair silicon with a metal halide perovskite are a promising option for surpassing the single-cell efficiency limit. We report a monolithic perovskite/silicon tandem with a certified power conversion efficiency of 29.15%.

Water Adsorption Enhances Electrical Conductivity in Transparent P-Type CuI.

CuI has been recently rediscovered as a p-type transparent conductor with a high figure of merit. Even though many metal iodides are hygroscopic, the effect of moisture on the electrical properties of CuI has not been clarified. In this work, we observe a 2-fold increase in the conductivity of CuI after exposure to ambient humidity for 5 h, followed by slight long-term degradation.

Microscopic origins of performance losses in highly efficient Cu(In,Ga)Se thin-film solar cells.

Thin-film solar cells based on polycrystalline absorbers have reached very high conversion efficiencies of up to 23-25%. In order to elucidate the limiting factors that need to be overcome for even higher efficiency levels, it is essential to investigate microscopic origins of loss mechanisms in these devices. In the present work, a high efficiency (21% without anti-reflection coating) copper indium gallium diselenide (CIGSe) solar cell is characterized by means of a correlative microscopy approach and corroborated by means of photoluminescence spectroscopy.

Assessment of a W:BiVO-CuBiOTandem Photoelectrochemical Cell for Overall Solar Water Splitting.

We assess a tandem photoelectrochemical cell consisting of a W:BiVO photoanode top absorber and a CuBiO photocathode bottom absorber for overall solar water splitting. We show that the W:BiVO photoanode oxidizes water and produces oxygen at potentials ≥0.7 V vs RHE when CoPi is added as a cocatalyst.