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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. Ministry of Education (MOE) Published version This work was supported by the Engineering and Physical Sciences Research Council (EPSRC) (EP/T005491/1 and EP/S023836/1). The authors also appreciate the support from the North East Centre for Energy Materials (NECEM) (EP/ R021503/1) and the British Council Newton Fund Institutional Links Grant (CRP01286). This research was funded by the Ministry of Education, Singapore Tier 2 MOE2019-T2-2- 066.

Aluminium-doped zinc oxide (AZO) is a potential low-cost alternative to indium tin oxide (ITO) for application in optoelectronic devices as a transparent conducting thin film. Typically, AZO thin films are deposited using expensive, high vacuum equipment with high energy cost and materials wastage. In this study, slot-die coating was used as an inexpensive alternative to vacuum deposition to form AZO nanoparticle thin films under ambient laboratory conditions. The films were characterised structurally, optically and electrically and compared with a commercially obtained AZO film fabricated using physical vapour deposition (PVD). Structural characterisation of the nanoparticle film shows uniform coverage across the substrate with increased crystal quality following annealing in Ar up to 500 $$^{\circ }$$ ∘ C. The optical properties of the nanoparticle film exhibit a wider band gap than the PVD film, while the high density of grain boundary defects between the nanoparticles inhibits sheet conductivity. Graphical abstract

Cu 2ZnSn(S,Se) 4 (CZTSSe) is a promising material for thin-film photovoltaics, however, the open-circuit voltage ( V OC) 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 Cu 2ZnSnS 4 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 V OC 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.

Earth abundant Cu