For halide perovskite solar cells (PSCs) to fulfill their vast potential for combining low-cost, high efficiency, and high throughput production they must be scaled using a truly transformative method, such as roll-to-roll processing. Bringing this reality closer to fruition, the present work demonstrates flexible perovskite solar cells with 18.1% power conversion efficiency on flexible Willow Glass substrates. We highlight the importance of the transparent conductive oxide (TCO) layers on device performance by studying various TCOs. While tin-doped indium oxide (ITO) and indium zinc oxide (IZO) based PSC devices demonstrate high photovoltaic performances, aluminum-doped zinc oxide (AZO) based devices underperformed in all device parameters. Analysis of X-ray photoemission spectroscopy data shows that the stoichiometry of the perovskite film surface changes dramatically when it is fabricated on AZO, demonstrating the importance of the substrate in perovskite film formation.
Al doped ZnO films have been grown by pulsed laser deposition (PLD) technique using ceramic targets sintered at different temperatures in the range 800 o C to 1400 o C. The effect of target sintering temperature on the structural, optical and electrical properties of the AZO films has been investigated. The X-ray diffraction (XRD) patterns show that besides the major hexagonal wurtzite phase of ZnO, the zinc aluminate (ZnAl 2 O 4 ) spinel impurity phase is present predominantly in the targets sintered at 900 o C onwards. The XRD peak intensity of the spinel phase increases as the sintering temperature increases. Although, no such impurity has been primarily appeared in the XRD pattern of the films deposited from these targets, the presence of a probable spinel phase has been sensed by the X-ray photoelectron spectroscopy (XPS) measurements. All the films show more than 90% transparency in the region 500 nm to 1400 nm.The electrical resistance of the target pellets also decreases with an increase in the sintering temperature up to 1100 o C and then increases. Similarly, the carrier concentration increases and the resistivity decreases with the sintering temperature attaining the values of 6.36×10 20 cm -3 and 6.38×10 -4 ohm-cm respectively for the films ablated from the targets sintered at temperatures 1000 o C (AZO1000) and 1100 o C (AZO1100) beyond which both the values deteriorate. An increase in the carrier concentration value is assigned to the modification of the grain boundaries by the spinel phase. Vacuum annealing of AZO1000 film at 350 o C results in a further increase in the carrier concentration to a value of 1×10 21 cm -3 . This film has been applied as a transparent electrode without texturing for a-Si:H solar cell which shows a conversion efficiency of ~3.93%.Our study for the first time shows that the presence of a ZnAl 2 O 4 phase to a certain extent in AZO film rather helps to achieve higher carrier concentration.
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