Manuel Kober-Czerny

Abstract:

Performance losses in positive–intrinsic–negative architecture perovskite solar cells are dominated by nonradiative recombination at the perovskite/organic electron transport layer interface, which is particularly problematic for wider bandgap perovskites. Large endeavours have been dedicated to the replacement of fullerenes, which are the most commonly used class of electron transport layers, with limited success thus far. In this work, we demonstrate blending the fullerene derivatives [6,6]-phenyl C61 butyric acid methyl ester (PCBM) and indene-C60 bis-adduct (ICBA) as a thin interlayer between 1.77 eV bandgap perovskite and an evaporated C60 layer. By tuning the fullerene blend to a trace 2% by mass of PCBM in ICBA, we remarkably form an interlayer which features improved energetic alignment with the perovskite and the PCBM : ICBA fullerene mixture, together with a stronger molecular ordering and an order of magnitude higher electron mobility than either neat PCBM or ICBA. Additional molecular surface passivation approaches are found to be beneficial in conjunction with this approach, resulting in devices with 19.5% steady state efficiency, a fill factor of 0.85 and an open-circuit voltage of 1.33 V, which is within 10% of the radiative limit of the latter two device parameters for this bandgap. This work highlights the complex nonlinear energetic behaviour with fullerene mixing, and how control of the energetics and crystallinity of these materials is crucial in overcoming the detrimental recombination losses that have historically limited perovskite solar cells.

Abstract:

Narrow bandgap lead-tin perovskites are essential components of next-generation all-perovskite multi-junction solar cells. However, their poor stability under operating conditions hinders successful implementation. In this work, we systematically investigate the underlying mechanisms of this instability under combined heat and light stress (ISOS L-2 conditions) by measuring changes in phase, conductivity, recombination and current-voltage characteristics. We find an increased impact of the redistribution of mobile ions during device operation to be the primary driver of performance loss during stressing, with further losses caused by a slower increase in non-radiative recombination and background hole density. Crucially, the dominant degradation mode changes with different hole transport materials, which we attribute to variations in iodine vacancy generation rates. By quantifying the impact of these mechanisms on device performance, we provide critical insights for improving the operational stability of lead-tin perovskite solar cells.

Abstract:

<jats:title>Abstract</jats:title><jats:p>2D lead halide perovskites (2DPs) offer chemical compatibility with 3D perovskites and enhanced stability, which are attractive for applications in photovoltaic and light‐emitting devices. However, such lowered structural dimensionality causes increased excitonic effects and highly anisotropic charge‐carrier transport. Determining the diffusivity of excitations, in particular for out‐of‐plane or inter‐layer transport, is therefore crucial, yet challenging to achieve. Here, an effective method is demonstrated for monitoring inter‐layer diffusion of photoexcitations in (PEA)<jats:sub>2</jats:sub>PbI<jats:sub>4</jats:sub> thin films by tracking time‐dependent changes in photoluminescence spectra induced by photon reabsorption effects. Selective photoexcitation from either substrate‐ or air‐side of the films reveals differences in diffusion dynamics encountered through the film profile. Time‐dependent diffusion coefficients are extracted from spectral dynamics through a 1D diffusion model coupled with an interference correction for refractive index variations arising from the strong excitonic resonance of 2DPs. Such analysis, together with structural probes, shows that minute misalignment of 2DPs planes occurs at distances far from the substrate, where efficient in‐plane transport consequently overshadows the less efficient out‐of‐plane transport in the direction perpendicular to the substrate. Through detailed analysis, a low out‐of‐plane excitation diffusion coefficient of (0.26 ± 0.03) ×10<jats:sup>−4</jats:sup> cm<jats:sup>2</jats:sup> s<jats:sup>−1</jats:sup> is determined, consistent with a diffusion anisotropy of ≈4 orders of magnitude.</jats:p>

Abstract:

<jats:p>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 that 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 halfstacks, 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 experimental data. Finally, we estimate mobility values for vertical charge-carrier transport, which is 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 for 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 can be expanded to a variety of other analysis techniques and that our method will be applicable to other semiconductors.</jats:p> <jats:sec> <jats:title/> <jats:supplementary-material> <jats:permissions> <jats:copyright-statement>Published by the American Physical Society</jats:copyright-statement> <jats:copyright-year>2025</jats:copyright-year> </jats:permissions> </jats:supplementary-material> </jats:sec>

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.