Crystalline Antimony Selenide Thin Films for Optoelectronics through Photonic Curing.

Thermal annealing is the most common postdeposition technique used to crystallize antimony selenide (Sb2Se3) thin films. However, due to slow processing speeds and a high energy cost, it is incompatible with the upscaling and commercialization of Sb2Se3 for future photovoltaics. Herein, for the first time, a fast-annealing technique that uses millisecond light pulses to deliver energy to the sample is adapted to cure thermally evaporated Sb2Se3 films. This study demonstrates how photonic curing (PC) conditions affect the outcome of Sb2Se3 phase conversion from amorphous to crystalline by evaluating the films' crystalline, morphological, and optical properties. We show that Sb2Se3 is readily converted under a variety of different conditions, but the zone where suitable films for optoelectronic applications are obtained is a small region of the parameter space. Sb2Se3 annealing with short pulses (<3 ms) shows significant damage to the sample, while using longer pulses (>5 ms) and a 4-5 J cm-2 radiant energy produces (211)- and (221)-oriented crystalline Sb2Se3 with minimal to no damage to the sample. A proof-of-concept photonically cured Sb2Se3 photovoltaic device is demonstrated. PC is a promising annealing method for large-area, high-throughput annealing of Sb2Se3 with various potential applications in Sb2Se3 photovoltaics.

Effect of metal dopants on the electrochromic performance of hydrothermally-prepared tungsten oxide materials.

Electrochromic (EC) glass has the potential to significantly improve energy efficiency in buildings by controlling the amount of light and heat that the building exchanges with its exterior. However, the development of EC materials is still hindered by key challenges such as slow switching time, low coloration efficiency, short cycling lifetime, and material degradation. Metal doping is a promising technique to enhance the performance of metal oxide-based EC materials, where adding a small amount of metal into the host material can lead to lattice distortion, a variation of oxygen vacancies, and a shorter ion transfer path during the insertion and de-insertion process. In this study, we investigated the effects of niobium, gadolinium, and erbium doping on tungsten oxide using a single-step solvothermal technique. Our results demonstrate that both insertion and de-insertion current density of a doped sample can be significantly enhanced by metal elements, with an improvement of about 5, 4 and 3.5 times for niobium, gadolinium and erbium doped tungsten oxide, respectively compared to a pure tungsten oxide sample. Moreover, the colouration efficiency increased by 16, 9 and 24% when doping with niobium, gadolinium and erbium, respectively. These findings suggest that metal doping is a promising technique for improving the performance of EC materials and can pave the way for the development of more efficient EC glass for building applications.

Enhanced Carrier Collection in Cd/In-Based Dual Buffers in Kesterite Thin-Film Solar Cells from Nanoparticle Inks.

Increasing the power conversion efficiency (PCE) of kesterite Cu2ZnSn(S,Se)4 (CZTSSe) solar cells has remained challenging over the past decade, in part due to open-circuit voltage (VOC)-limiting defect states at the absorber/buffer interface. Previously, we found that substituting the conventional CdS buffer layer with In2S3 in CZTSSe devices fabricated from nanoparticle inks produced an increase in the apparent doping density of the CZTSSe film and a higher built-in voltage arising from a more favorable energy-band alignment at the absorber/buffer interface. However, any associated gain in VOC was negated by the introduction of photoactive defects at the interface. This present study incorporates a hybrid Cd/In dual buffer in CZTSSe devices that demonstrate an average relative increase of 11.5% in PCE compared to CZTSSe devices with a standard CdS buffer. Current density-voltage analysis using a double-diode model revealed the presence of (i) a large recombination current in the quasi-neutral region (QNR) of the CZTSSe absorber in the standard CdS-based device, (ii) a large recombination current in the space-charge region (SCR) of the hybrid buffer CZTSSe-In2S3-CdS device, and (iii) reduced recombination currents in both the QNR and SCR of the CZTSSe-CdS-In2S3 device. This accounts for a notable 9.0% average increase in the short-circuit current density (JSC) observed in CZTSSe-CdS-In2S3 in comparison to the CdS-only CZTSSe solar cells. Energy-dispersive X-ray, secondary-ion mass spectroscopy, and grazing-incidence X-ray diffraction compositional analysis of the CZTSSe layer in the three types of kesterite solar cells suggest that there is diffusion of elemental In and Cd into the absorbers with a hybrid buffer. Enhanced Cd diffusion concomitant with a double postdeposition heat treatment of the hybrid buffer layers in the CZTSSe-CdS-In2S3 device increases carrier collection and extraction and boosts JSC. This is evidenced by electron-beam-induced current measurements, where higher current generation and collection near to the p-n junction is observed, accounting for the increase in JSC in this device. It is expected that optimization of the heat treatment of the hybrid buffer layers will lead to further improvements in the device performance.

Ex situ Ge-doping of CZTS nanocrystals and CZTSSe solar absorber films.

Cu2ZnSn(S,Se)4 (CZTSSe) is a promising material for thin-film photovoltaics, however, the open-circuit voltage (VOC) deficit of CZTSSe prevents the device performance from exceeding 13% conversion efficiency. CZTSSe is a heavily compensated material that is rich in point defects and prone to the formation of secondary phases. The landscape of these defects is complex and some mitigation is possible by employing non-stoichiometric conditions. Another route used to reduce the effects of undesirable defects is the doping and alloying of the material to suppress certain defects and improve crystallization, such as with germanium. The majority of works deposit Ge adjacent to a stacked metallic precursor deposited by physical vapour deposition before annealing in a selenium rich atmosphere. Here, we use an established hot-injection process to synthesise Cu2ZnSnS4 nanocrystals of a pre-determined composition, which are subsequently doped with Ge during selenisation to aid recrystallisation and reduce the effects of Sn species. Through Ge incorporation, we demonstrate structural changes with a negligible change in the energy bandgap but substantial increases in the crystallinity and grain morphology, which are associated with a Ge-Se growth mechanism, and gains in both the VOC and conversion efficiency. We use surface energy-filtered photoelectron emission microscopy (EF-PEEM) to map the surface work function terrains and show an improved electronic landscape, which we attribute to a reduction in the segregation of low local effective work function (LEWF) Sn(II) chalcogenide phases.

Recovery Mechanisms in Aged Kesterite Solar Cells.

For successful long-term deployment and operation of kesterites Cu2ZnSn(S x Se1-x )4 (CZTSSe) as light-absorber materials for photovoltaics, device stability and recovery in kesterite solar cells are investigated. A low-temperature heat treatment is applied to overcome the poor charge extraction that developed in the natural aging process. It is suggested that defect states at aged CZTSSe/CdS heterojunctions were reduced, while apparent doping density in the CZTSSe absorber increased due to Cd/Zn interdiffusion at the heterojunction during the annealing process. In situ annealing experiments in a transmission electron microscope were used to investigate the elemental diffusion at the CZTSSe/CdS heterojunction. This study reveals the critical role of heat treatment to enhance the absorber/Mo back contact, improve the quality of the absorber/buffer heterojunction, and recover the device performance in aged kesterite thin-film solar cells.

Double-sided slippery liquid-infused porous materials using conformable mesh.

Often wetting is considered from the perspective of a single surface of a rigid substrate and its topographical properties such as roughness or texture. However, many substrates, such as membranes and meshes, have two useful surfaces. Such flexible substrates also offer the potential to be formed into structures with either a double-sided surface (e.g. by joining the ends of a mesh as a tape) or a single-sided surface (e.g. by ends with a half-twist). When a substrate possesses holes, it is also possible to consider how the spaces in the substrate may be connected or disconnected. This combination of flexibility, holes and connectedness can therefore be used to introduce topological concepts, which are distinct from simple topography. Here, we present a method to create a Slippery Liquid-Infused Porous Surface (SLIPS) coating on flexible conformable doubled-sided meshes and for coating complex geometries. By considering the flexibility and connectedness of a mesh with the surface properties of SLIPS, we show it is possible to create double-sided SLIPS materials with high droplet mobility and droplet control on both faces. We also exemplify the importance of flexibility using a mesh-based SLIPS pipe capable of withstanding laminar and turbulent flows for 180 and 90 minutes, respectively. Finally, we discuss how ideas of topology introduced by the SLIPS mesh might be extended to create completely new types of SLIPS systems, such as Mobius strips and auxetic metamaterials.