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Christoph J. Brabec

Publications and source records attributed to Christoph J. Brabec.

30 records · Page 2Linked to original sources

Power-law density of states in organic solar cells revealed by the open-circuit voltage dependence of the ideality factor

The density of states (DOS) is fundamentally important for understanding physical processes in organic disordered semiconductors, yet hard to determine experimentally. We evaluated the DOS by considering recombination via tail states and using the temperature and open-circuit voltage ($V_\mathrm{oc}$) dependence of the ideality factor in organic solar cells. By performing Suns-$V_\mathrm{oc}$ measurements, we find that gaussian and exponential distributions describe the DOS only at a given quasi-Fermi level splitting. The DOS width increases linearly with the DOS depth, revealing the power-law DOS in these materials.

physics.app-ph↗

Traps and transport resistance: the next frontier for stable state-of-the-art non-fullerene acceptor solar cells

Stability is one of the most important challenges facing organic solar cells (OSC) on their path to commercialization. In the high-performance material system PM6:Y6 studied here, investigate degradation mechanisms of inverted photovoltaic devices. We have identified two distinct degradation pathways: one requires presence of both illumination and oxygen and features a short-circuit current reduction, the other one is induced thermally and marked by severe losses of open-circuit voltage and fill factor. We focus our investigation on the thermally accelerated degradation. Our findings show that bulk material properties and interfaces remain remarkably stable, however, aging-induced defect state formation in the active layer remains the primary cause of thermal degradation. The increased trap density leads to higher non-radiative recombination, which limits open-circuit voltage and lowers charge carrier mobility in the photoactive layer. Furthermore, we find the trap-induced transport resistance to be the major reason for the drop in fill factor. Our results suggest that device lifetimes could be significantly increased by marginally suppressing trap formation, leading to a bright future for OSC.

cond-mat.mtrl-sci↗

Phase-field simulation of liquid-vapor equilibrium and evaporation of fluid mixtures

In solution-processing of thin films, the material layer is deposited from a solution composed of several solutes and solvents. The final morphology and hence the properties of the film often depend on the time needed for the evaporation of the solvents. This is typically the case for organic photoactive or electronic layers. Therefore, it is important to be able to predict the evaporation kinetics of such mixtures. We propose here a new phase-field model for the simulation of evaporating fluid mixtures and simulate their evaporation kinetics. Similar to the Hertz-Knudsen theory, the local liquid-vapor equilibrium is assumed to be reached at the film surface and evaporation is driven by diffusion away from this gas layer. In the situation where the evaporation is purely driven by the liquid-vapor equilibrium, the simulations match the behavior expected theoretically from the free energy: for evaporation of pure solvents, the evaporation rate is constant and proportional to the vaporpressure. For mixtures, the evaporation rate is in general strongly time-dependent because of the changing composition of the film. Nevertheless, for highly non-ideal mixtures, such as poorly compatible fluids or polymer solutions, the evaporation rate becomes almost constant in the limit of low Biot numbers. The results of the simulation have been successfully compared to experiments on a polystyrene-toluene mixture. The model allows to take into account deformations of the liquid-vapor interface and therefore to simulate film roughness or dewetting.

physics.app-ph↗

The Evolution of Materials Acceleration Platforms -- Towards the Laboratory of the Future with AMANDA

The development of complex functional materials poses a multi-objective optimization problem in a large multidimensional parameter space. Solving it requires reproducible, user independent laboratory work and intelligent preselection of experiments. However, experimental materials science is a field where manual routines are still predominant, although other domains like pharmacy or chemistry have long used robotics and automation. As the number of publications on Materials Acceleration Platforms (MAPs) increases steadily, we review selected systems and fit them into the stages of a general material development process to examine the evolution of MAPs. Subsequently we present our approach to laboratory automation in materials science. We introduce AMANDA (Autonomous Materials and Device Application Platform), a generic platform for distributed materials research comprising a self-developed software backbone and several MAPs. One of them, LineOne (L1), is specifically designed to produce and characterize solution processed thin-film devices like organic solar cells (OSC). It is designed to perform precise closed-loop screenings of up to 272 device variations per day yet allows further upscaling. Each individual solar cell is fully characterized and all process steps are comprehensively documented. We want to demonstrate the capabilities of AMANDA L1 with OSCs based on PM6:Y6 with 13.7% efficiency when processed in air. Further we discuss challenges and opportunities of highly automated research platforms and elaborate on the future integration of additional techniques, methods and algorithms in order to advance to fully autonomous self-optimizing systems - a paradigm shift in functional materials development leading to the laboratory of the future.

cond-mat.mtrl-sci↗

Joint Super-Resolution and Rectification for Solar Cell Inspection

Visual inspection of solar modules is an important monitoring facility in photovoltaic power plants. Since a single measurement of fast CMOS sensors is limited in spatial resolution and often not sufficient to reliably detect small defects, we apply multi-frame super-resolution (MFSR) to a sequence of low resolution measurements. In addition, the rectification and removal of lens distortion simplifies subsequent analysis. Therefore, we propose to fuse this pre-processing with standard MFSR algorithms. This is advantageous, because we omit a separate processing step, the motion estimation becomes more stable and the spacing of high-resolution (HR) pixels on the rectified module image becomes uniform w. r. t. the module plane, regardless of perspective distortion. We present a comprehensive user study showing that MFSR is beneficial for defect recognition by human experts and that the proposed method performs better than the state of the art. Furthermore, we apply automated crack segmentation and show that the proposed method performs 3x better than bicubic upsampling and 2x better than the state of the art for automated inspection.

cs.CV↗

Bridging the gap between photovoltaics R&D and manufacturing with data-driven optimization

Novel photovoltaics, such as perovskites and perovskite-inspired materials, have shown great promise due to high efficiency and potentially low manufacturing cost. So far, solar cell R&D has mostly focused on achieving record efficiencies, a process that often results in small batches, large variance, and limited understanding of the physical causes of underperformance. This approach is intensive in time and resources, and ignores many relevant factors for industrial production, particularly the need for high reproducibility and high manufacturing yield, and the accompanying need of physical insights. The record-efficiency paradigm is effective in early-stage R&D, but becomes unsuitable for industrial translation, requiring a repetition of the optimization procedure in the industrial setting. This mismatch between optimization objectives, combined with the complexity of physical root-cause analysis, contributes to decade-long timelines to transfer new technologies into the market. Based on recent machine learning and technoeconomic advances, our perspective articulates a data-driven optimization framework to bridge R&D and manufacturing optimization approaches. We extend the maximum-efficiency optimization paradigm by considering two additional dimensions: a technoeconomic figure of merit and scalable physical inference. Our framework naturally aligns different stages of technology development with shared optimization objectives, and accelerates the optimization process by providing physical insights.

physics.app-ph↗

A phase-field model for the evaporation of thin film mixtures

The performance of solution-processed solar cells strongly depends on the geometrical structure and roughness of the photovoltaic layers formed during film drying. During the drying process, the interplay of crystallization and liquid-liquid demixing leads to the structure formation on the nano- and microscale and to the final rough film. In order to better understand how the film structure can be improved by process engineering, we aim at theoretically investigating these systems by means of phase-field simulations. We introduce an evaporation model based on the Cahn-Hilliard equation for the evolution of the fluid concentrations coupled to the Allen-Cahn equation for the liquid-vapour phase transformation. We demonstrate its ability to match the experimentally measured drying kinetics and study the impact of the parameters of our model. Furthermore, the evaporation of solvent blends and solvent-vapour annealing are investigated. The dry film roughness emerges naturally from our set of equations, as illustrated through preliminary simulations of spinodal decomposition and film drying on structured substrates.

physics.app-ph↗

Light Intensity Modulated Impedance Spectroscopy (LIMIS) in All-Solid-State Solar Cells at Open Circuit

Potentiostatic impedance spectroscopy (IS) is a well stablished characterization technique for elucidating the electric resistivity and capacitive features of materials and devices. In the case of solar cells, by applying a small voltage perturbation the current signal is recorded and the recombination processes and defect distributions are among the typical outcomes in IS studies. In this work a photo-impedance approach, named light intensity modulated impedance spectroscopy (LIMIS), is first tested in all-solid-state photovoltaic cells by recording the individual photocurrent (IMPS) and photovoltage (IMVS) responsivity signals due to a small light perturbation at open-circuit (OC), and combining them: LIMIS=IMVS/IMPS. The experimental LIMIS spectra from silicon, organic, and perovskite solar cells are presented and compared with IS. An analysis of the equivalent circuit numerical models for total resistive and capacitive features is discussed. Our theoretical findings show a correction to the lifetimes evaluations by obtaining the total differential resistances and capacitances combining IS and LIMIS measurements. This correction addresses the discrepancies among different techniques, as shown with transient photovoltage. The experimental differences between IS and LIMIS (i) proves the unviability of the superposition principle, (ii) suggest a bias-dependent photo-current correction to the empirical Shockley equation of the steady-state current at different illumination intensities around OC and (iii) are proposed as a potential figure of merit for characterizing performance and stability of solar cells. In addition, new features are reported for the low-frequency capacitance of perovskite solar cells, measured by IS and LIMIS.

physics.app-ph↗

Analytical Model for Light Modulating Impedance Spectroscopy (LIMIS) in All-Solid-State p-n Junction Solar Cells at Open-Circuit

Non-circuit theory drift-diffusion numerical simulation of standard potentiostatic impedance spectroscopy (IS) is a well-known strategy for characterization of materials and electronic devices. It implies the time-dependent solutions from the continuity and Poisson's equations under small perturbation of the bias boundary condition at the electrodes. But in the case of photo-sensitive devices a small light perturbation can be also taken modulating the generation rate along the absorber bulk. In that focus, this work approaches a set of analytical solutions for the signals of IS and intensity modulated photocurrent and photovoltage spectroscopies, IMPS and IMVS respectively, from one-sided p-n junction solar cells at open-circuit. Subsequently, a photo-impedance signal named light intensity modulated impedance spectroscopy (LIMIS equals IMVS over IMPS) is analytically simulated and its difference with respect to IS suggests a correlation with the surface charge carrier recombination velocity. This is an illustrative result and starting point for future more realistic numerical simulations.

cond-mat.mtrl-sci↗

Embedding Physics Domain Knowledge into a Bayesian Network Enables Layer-by-Layer Process Innovation for Photovoltaics

Process optimization of photovoltaic devices is a time-intensive, trial and error endeavor, without full transparency of the underlying physics, and with user-imposed constraints that may or may not lead to a global optimum. Herein, we demonstrate that embedding physics domain knowledge into a Bayesian network enables an optimization approach that identifies the root cause(s) of underperformance with layer by-layer resolution and reveals alternative optimal process windows beyond global black-box optimization. Our Bayesian-network approach links process conditions to materials descriptors (bulk and interface properties, e.g., bulk lifetime, doping, and surface recombination) and device performance parameters (e.g., cell efficiency), using a Bayesian inference framework with an autoencoder-based surrogate device-physics model that is 100x faster than numerical solvers. With the trained surrogate model, our approach is robust and reduces significantly the time consuming experimentalist intervention, even with small numbers of fabricated samples. To demonstrate our method, we perform layer-by-layer optimization of GaAs solar cells. In a single cycle of learning, we find an improved growth temperature for the GaAs solar cells without any secondary measurements, and demonstrate a 6.5% relative AM1.5G efficiency improvement above baseline and traditional black-box optimization methods.

physics.app-ph↗

Beyond Ternary OPV: High-Throughput Experimentation and Self-Driving Laboratories Optimize Multi-Component Systems

Fundamental advances to increase the efficiency as well as stability of organic photovoltaics (OPVs) are achieved by designing ternary blends which represents a clear trend towards multi-component active layer blends. We report the development of high-throughput and autonomous experimentation methods for the effective optimization of multi-component polymer blends for OPVs. A method for automated film formation enabling the fabrication of up to 6048 films per day is introduced. Equipping this automated experimentation platform with a Bayesian optimization, a self-driving laboratory is constructed that autonomously evaluates measurements to design and execute the next experiments. To demonstrate the potential of these methods, a four-dimensional parameter space of quaternary OPV blends is mapped and optimized for photo-stability. While with conventional approaches roughly 100 mg of material would be necessary, the robot based platform can screen 2,000 combinations with less than 10 mg and machine learning enabled autonomous experimentation identifies the stable compositions with less than 1 mg.

physics.app-ph↗

Fast and robust detection of solar modules in electroluminescence images

Fast, non-destructive and on-site quality control tools, mainly high sensitive imaging techniques, are important to assess the reliability of photovoltaic plants. To minimize the risk of further damages and electrical yield losses, electroluminescence (EL) imaging is used to detect local defects in an early stage, which might cause future electric losses. For an automated defect recognition on EL measurements, a robust detection and rectification of modules, as well as an optional segmentation into cells is required. This paper introduces a method to detect solar modules and crossing points between solar cells in EL images. We only require 1-D image statistics for the detection, resulting in an approach that is computationally efficient. In addition, the method is able to detect the modules under perspective distortion and in scenarios, where multiple modules are visible in the image. We compare our method to the state of the art and show that it is superior in presence of perspective distortion while the performance on images, where the module is roughly coplanar to the detector, is similar to the reference method. Finally, we show that we greatly improve in terms of computational time in comparison to the reference method.

cs.CV↗