Akash Dasgupta

Abstract:

High-efficiency solar cell architectures, including silicon heterojunction (SHJ) and perovskite/silicon tandems, rely heavily on the unique properties of transparent conducting oxides (TCOs). The push towards terawatt-scale PV manufacturing means it is increasingly desirable to develop indium-free TCOs to facilitate the upscaled manufacturing of high-efficiency cell designs. Aluminium-doped ZnO (AZO) deposited by atomic layer deposition (ALD) has emerged as a promising candidate due to its combination of optical transparency and electrical conductivity. In addition, AZO has also been shown to passivate the c-Si surface. The ability for one material to provide all three properties without requiring any indium is advantageous in single junction and tandem solar devices. Herein, we demonstrate exceptional silicon surface passivation using AZO/AlOx stacks deposited with ALD, with a J0 < 1 fA cm−2 and corresponding implied open circuit voltage (iVOC) of 740 mV. We provide a comprehensive analysis of the role of ALD precursor dosing to achieve optimised performance. A broad range of characterisation approaches were used to probe the structural, compositional, and chemical properties of AZO films. These indicated that the passivation properties are governed by a delicate interplay between the Zn and Al concentrations in the film, highlighting the importance of precise process control. Optical modelling in a single junction SHJ architecture indicates these AZO films are close in performance to high-mobility indium-containing TCOs. The insights provided by this work may help to further the case of indium-free TCOs, which is critical for upscaled production of high-efficiency solar cells.

Abstract:

In this work we demonstrate that time-resolved photoluminescence data of metal halide perovskites can be effectively evaluated by combining Bayesian inference with a Markov-Chain Monte-Carlo algorithm and a physical model. This approach enables us to infer a high number of parameters which govern the performance of metal halide perovskite-based devices, alongside the probability distributions of those parameters, as well as correlations among all parameters. Via studying a set of "half-stacks’‘, comprising electron and hole transport materials contacting perovskite thin-films, we determine surface recombination velocities at these interfaces with high precision. From the probability distributions of all inferred parameters, we can simulate intensity-dependent photoluminescence quantum efficiency and compare it to the experimental data. Finally, we estimate mobility values for the "vertical’’ charge carrier transport, that perpendicular to the plane of the substrate, for all samples using our approach. Since this mobility estimation is derived from charge carrier diffusion over the length-scale of the film thickness and in the vertical direction, it is highly relevant to transport in photovoltaic and light emitting devices. Our approach of coupling spectroscopic measurements with advanced, computational analysis will help speed up scientific research in the field of optoelectronic materials and devices and exemplifies how carefully constructed computational algorithms can derive valuable plurality of information from simple datasets. We expect that our approach will be expandable to a variety of other analysis techniques and that our method will be applicable to other semiconductors.

Abstract:

Abstract:

All data reported in publication: Impact of precursor dosing on the surface passivation of AZO/AlOx stacks formed using atomic layer deposition

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.