Grey Christoforo PhD

Abstract:

Transparent conductive films are key components of many optoelectronic devices but are often made from either scarce or brittle materials like indium tin oxide. Carbon nanotube-polymer films offer an abundant and flexible alternative. Here, we report how the dimensions of the carbon nanotube raw material affect their thin film performance and thickness yield when processed with the polymer ethylene-vinyl acetate. We perform chemical doping with several halogenated metals and find the electron affinity of the metal to be a good indicator of p-doping effectiveness. We identify CuCl2 as low-cost alternative to the established gold chloride dopants. Optimising the dopant deposition method allows us to reduce the effect of doping on the optical transmittance. Percolation analysis of our films demonstrates that optimized single-walled carbon nanotube-ethylene-vinyl acetate films show no sign of percolation effects down to thicknesses of 5 nm. Finally, we produce transparent touch-sensitive devices. Comparing several of these devices, we find a linear relationship between the sheet resistance and the on/off ratio of the touch sensing that can be used to determine a threshold film thickness. Using doped carbon nanotube-ethylene-vinyl acetate films increases the on/off ratio and allows us to fabricate touch-sensitive devices with an on/off ratio of 10 at 95% optical transmittance. This clearly demonstrates the potential of these films for transparent touch-sensitive applications.

Abstract:

Vacuum deposition of metal halide perovskite is a scalable and adaptable method. In this study, we adopt sequential evaporation to form the perovskite layer and reveal how the relative humidity during the annealing step, impacts its crystallinity and the photoluminescence quantum yield (PLQY). By controlling the humidity, we achieved a significant enhancement of 50 times in PLQY from 0.12% to 6%. This improvement corresponds to an increase in implied open-circuit voltage (Voc) of over 100 meV. We investigate the origin of this enhanced PLQY by combining structural, chemical and spectroscopic methods. Our results show that annealing in a controlled humid environment improves the organic and inorganic halides' interdiffusion throughout the bulk, which in turn significantly reduces non-radiative recombination both in the bulk and at the interfaces with the charge transport layers, which enhanced both the attainable open-circuit voltage and the charge carrier diffusion length. We further demonstrate that the enhanced intermixing results in fully vacuum-deposited FA0.85Cs0.15Pb(IxCl1−x)3 p-i-n perovskite solar cells (PSCs) with a maximum power point tracked efficiency of 21.0% under simulated air mass (AM) 1.5G 100 mW cm−2 irradiance. Additionally, controlled humidity annealed PSCs exhibit superior stability when aged under full spectrum simulated solar illumination at 85 °C and in open-circuit conditions.

Abstract:

Multijunction photovoltaics (PVs) are gaining prominence owing to their superior capability of achieving power conversion efficiencies (PCEs) beyond the radiative limit of single-junction cells^1-8, where improving narrow bandgap tin-lead perovskites is critical for thin-film devices⁹. With a focus on understanding the chemistry of tin-lead perovskite precursor solutions, we herein find that Sn(II) species dominate interactions with precursors and additives and uncover the exclusive role of carboxylic acid in regulating solution colloidal properties and film crystallisation, and ammonium in improving film optoelectronic properties. Materials that combine these two function groups, amino acid salts, considerably improve the semiconducting quality and homogeneity of perovskite films, surpassing the effect of the individual functional groups when introduced as part of separate molecules. Our enhanced tin-lead perovskite layer allows us to fabricate solar cells with PCEs of 23.9, 29.7 (certified 29.26%), and 28.7% for single-, double-, and triple-junction devices, respectively. Our 1-cm² triple-junction devices show PCEs of 28.4% (certified 27.28%). Encapsulated triple-junction cells maintain 80% of their initial efficiencies after 860 h maximum power point tracking in ambient. We further fabricate quadruple-junction devices and obtain PCEs of 27.9% with the highest open-circuit voltage of 4.94 V. This work establishes a new benchmark for multijunction PVs.

Abstract:

Perovskite solar cells (PSCs) offer an efficient, inexpensive alternative to current photovoltaic technologies, with the potential for manufacture via high-throughput coating methods. However, challenges for commercial-scale solution-processing of metal-halide perovskites include the use of harmful solvents, the expense of maintaining controlled atmospheric conditions, and the inherent instabilities of PSCs under operation. Here, we address these challenges by introducing a high volatility, low toxicity, biorenewable solvent system to fabricate a range of 2D perovskites, which we use as highly effective precursor phases for subsequent transformation to α-formamidinium lead triiodide (α-FAPbI3), fully processed under ambient conditions. PSCs utilising our α-FAPbI3 reproducibly show remarkable stability under illumination and elevated temperature (ISOS-L-2) and “damp heat” (ISOS-D-3) stressing, surpassing other state-of-the-art perovskite compositions. We determine that this enhancement is a consequence of the 2D precursor phase crystallisation route, which simultaneously avoids retention of residual low-volatility solvents (such as DMF and DMSO) and reduces the rate of degradation of FA+ in the material. Our findings highlight both the critical role of the initial crystallisation process in determining the operational stability of perovskite materials, and that neat FA+-based perovskites can be competitively stable despite the inherent metastability of the α-phase.

Abstract:

As perovskite photovoltaics stride towards commercialization, reverse bias degradation in shaded cells that must current match illuminated cells is a serious challenge. Previous research has emphasized the role of iodide and silver oxidation, and the role of hole tunnelling from the electron-transport layer into the perovskite to enable the flow of current under reverse bias in causing degradation. Here we show that device architecture engineering has a significant impact on the reverse bias behaviour of perovskite solar cells. By implementing both a ~35-nm-thick conjugated polymer hole transport layer and a more electrochemically stable back electrode, we demonstrate average breakdown voltages exceeding −15 V, comparable to those of silicon cells. Our strategy for increasing the breakdown voltage reduces the number of bypass diodes needed to protect a solar module that is partially shaded, which has been proven to be an effective strategy for silicon solar panels.