Bypassing the Single Junction Limit with Advanced Photovoltaic Architectures.

Multijunction devices and photon up- and down-conversion are prominent concepts aimed at increasing photovoltaic efficiencies beyond the single junction limit. Integrating these concepts into advanced architectures may address long-standing issues such as processing complexity, microstructure control, and resilience against spectral changes of the incoming radiation. However, so far, no models have been established to predict the performance of such integrated architectures. Here, a simulation environment based on Bayesian optimization is presented, that can predict and virtually optimize the electrical performance of multi-junction architectures, both vertical and lateral, in combination with up- and down-conversion materials. Microstructure effects on performance are explicitly considered using machine-learned predictive models from high throughput experimentation on simpler architectures. Two architectures that would surpass the single junction limit of photovoltaic energy conversion at reasonable complexity are identified: a vertical "staggered half octave system," where selective absorption allows the use of 6 different bandgaps, and the lateral "overlapping rainbow system" where selective irradiation allows the use of a narrowband energy acceptor with reduced voltage losses, according to the energy gap law. Both architectures would be highly resilient against spectral changes, in contrast with two terminal multi-junction architectures which are limited by Kirchhoff's law.

Understanding Causalities in Organic Photovoltaics Device Degradation in a Machine-Learning-Driven High-Throughput Platform.

Organic solar cells (OSCs) now approach power conversion efficiencies of 20%. However, in order to enter mass markets, problems in upscaling and operational lifetime have to be solved, both concerning the connection between processing conditions and active layer morphology. Morphological studies supporting the development of structure-process-property relations are time-consuming, complex, and expensive to undergo and for which statistics, needed to assess significance, are difficult to be collected. This work demonstrates that causal relationships between processing conditions, morphology, and stability can be obtained in a high-throughput method by combining low-cost automated experiments with data-driven analysis methods. An automatic spectral modeling feeds parametrized absorption data into a feature selection technique that is combined with Gaussian process regression to quantify deterministic relationships linking morphological features and processing conditions with device functionality. The effect of the active layer thickness and the morphological order is further modeled by drift-diffusion simulations and returns valuable insight into the underlying mechanisms for improving device stability by tuning the microstructure morphology with versatile approaches. Predicting microstructural features as a function of processing parameters is decisive know-how for the large-scale production of OSCs.

Influence of tin oxide decoration on the junction conductivity of silver nanowires.

Flexible electrodes using nanowires (NWs) suffer from challenges of long-term stability and high junction resistance which limit their fields of applications. Welding via thermal annealing is a common strategy to enhance the conductivity of percolated NW networks, however, it affects the structural and mechanical integrity of the NWs. In this study we show that the decoration of NWs with an ultrathin metal oxide is a potential alternative procedure which not only enhances the thermal and chemical stability but, moreover, provides a totally different mechanism to reduce the junction resistance upon heat treatment. Here, we analyze the effect of SnOxdecoration on the conductance of silver NWs and NW junctions by using a four-probe measurement setup inside a scanning electron microscope. Dedicated transmission electron microscopy analysis in plan-view and cross-section geometry are carried out to characterize the nanowires and the microstructure of the junctions. Upon heat treatment the junction resistance of both plain silver NWs and SnOx-decorated NWs is reduced by around 80%. While plain silver NWs show characteristic junction welding during annealing, the SnOx-decoration reduces junction resistance by a solder-like process which does not affect the mechanical integrity of the NW junction and is therefore expected to be superior for applications.

Understanding the Microstructure Formation of Polymer Films by Spontaneous Solution Spreading Coating with a High-Throughput Engineering Platform.

An important step of the great achievement of organic solar cells in power conversion efficiency is the development of low-band gap polymer donors, PBDB-T derivatives, which present interesting aggregation effects dominating the device performance. The aggregation of polymers can be manipulated by a series of variables from a materials design and processing conditions perspective; however, optimization of film quality is a time- and energy-consuming work. Here, we introduce a robot-based high-throughput platform (HTP) that is offering automated film preparation and optical spectroscopy thin-film characterization in combination with an analysis algorithm. PM6 films are prepared by the so-called spontaneous film spreading (SFS) process, where a polymer solution is coated on a water surface. Automated acquisition of UV/Vis and photoluminescence (PL) spectra and automated extraction of morphological features is coupled to Gaussian Process Regression to exploit available experimental evidence for morphology optimization but also for hypothesis formulation and testing with respect to the underlying physical principles. The integrated spectral modeling workflow yields quantitative microstructure information by distinguishing amorphous from ordered phases and assesses the extension of amorphous versus the ordered domains. This research provides an easy to use methodology to analyze the exciton coherence length in conjugated semiconductors and will allow to optimize exciton splitting in thin film organic semiconductor layers as a function of processing.

A Generalized Crystallization Protocol for Scalable Deposition of High-Quality Perovskite Thin Films for Photovoltaic Applications.

Metal halide perovskite solar cells (PSCs) have raised considerable scientific interest due to their high cost-efficiency potential for photovoltaic solar energy conversion. As PSCs already are meeting the efficiency requirements for renewable power generation, more attention is given to further technological barriers as environmental stability and reliability. However, the most major obstacle limiting commercialization of PSCs is the lack of a reliable and scalable process for thin film production. Here, a generic crystallization strategy that allows the controlled growth of highly qualitative perovskite films via a one-step blade coating is reported. Through rational ink formulation in combination with a facile vacuum-assisted precrystallization strategy, it is possible to produce dense and uniform perovskite films with high crystallinity on large areas. The universal application of the method is demonstrated at the hand of three typical perovskite compositions with different band gaps. P-i-n perovskite solar cells show fill factors up to 80%, underpinning the statement of the importance of controlling crystallization dynamics. The methodology provides important progress toward the realization of cost-effective large-area perovskite solar cells for practical applications.

Time-Resolved Analysis of Dielectric Mirrors for Vapor Sensing.

Dielectric mirrors based on bilayers of polystyrene- block-poly(ethylene- ran-butylene)- block-polystyrene (SEBS) and poly(vinyl alcohol) (PVA)-zirconium dioxide (ZrO2) nanocomposites are fabricated for vapor sensing. When exposed to specific solvent vapor, the layers of dielectric mirrors can gradually swell and cause a red-shift of the reflection band. Because PVA solely responds to water and SEBS is sensitive to several different types of organic solvents, the mirrors can respond to a large variety of solvents. The dual-functional hydrophilic ZrO2 nanoparticles are introduced to not only enlarge the refractive index contrast but also increase the permeability. Time-resolved measurements show that mirrors with nanoparticles have a significantly faster response than those without nanoparticles. Moreover, the dependence on relative humidity is studied for representative solvents, and several types of solvents are selected to show the dependence on the solvent-polymer interaction parameters at typical relative humidity, which allows one to predict the responsivity and selectivity of the sensors.

Detailed optical modelling and light-management of thin-film organic solar cells with consideration of small-area effects.

We present detailed numerical and experimental investigation of thin-film organic solar cells with a micro-textured light management foil applied on top of the front glass substrate. We first demonstrate that measurements of small-area laboratory solar cells are susceptible to a significant amount of optical losses that could lead to false interpretation of the measurement results. Using the combined optical model CROWM calibrated with realistic optical properties of organic films and other layers, we identify the origins of these losses and quantify the extent of their influence. Further on, we identify the most important light management mechanisms of the micro-textured foil, among which the prevention of light escaping at the front side of the cell is revealed as the dominant one. Detailed three-dimensional simulations show that the light-management foil applied on top of a large-area organic solar cell can reduce the total reflection losses by nearly 60% and improve the short-circuit current density by almost 20%. Finally, by assuming realistic open-circuit voltage and especially the realistic fill factor that deteriorates as the absorber layer thickness is increased, we determine the optimal absorber layer thickness that would result in the highest power conversion efficiency of the investigated organic solar cells.

The fabrication of color-tunable organic light-emitting diode displays via solution processing.

Electroluminescent devices based on organic semiconductors have attracted significant attention owing to their promising applications in flat-panel displays. The conventional display pixel consisting of side-by-side arrayed red, green and blue subpixels represents the mature technology but bears an intrinsic deficiency of a low pixel density. Constructing an individual color-tunable pixel that comprises vertically stacked subpixels is considered an advanced technology. Although color-tunable organic light-emitting diodes (OLEDs) have been fabricated using the vacuum deposition of small molecules, the solution processing of conjugated polymers would enable a much simpler and inexpensive manufacturing process. Here we present the all-solution processing of color-tunable OLEDs comprising two vertically stacked polymer emitters. A thin layer of highly conducting and transparent silver nanowires is introduced as the intermediate charge injection contact, which allows the emission spectrum and intensity of the tandem devices to be seamlessly manipulated. To demonstrate a viable application of this technology, a 4-by-4 pixelated matrix color-tunable display was fabricated.

Overcoming the Interface Losses in Planar Heterojunction Perovskite-Based Solar Cells.

A scalable, hysteresis-free and planar architecture perovskite solar cell is presented, employing a flame spray synthesized low-temperature processed NiO (LT-NiO) as hole-transporting layer yielding efficiencies close to 18%. Importantly, it is found that LT-NiO boosts the limits of open-circuit voltages toward an impressive non-radiative voltage loss of 0.226 V only, whereas PEDOT: PSS suffers from significant large non-radiative recombination losses.

Coloring Semitransparent Perovskite Solar Cells via Dielectric Mirrors.

While perovskite-based semitransparent solar cells for window applications show competitive levels of transparency and efficiency compared to organic photovoltaics, the color perception of the perovskite films is highly restricted because band gap engineering results in losses in power conversion efficiencies. To overcome the limitation in visual aesthetics, we combined semitransparent perovskite solar cells with dielectric mirrors. This approach enables one to tailor the device appearance to almost any desired color and simultaneously offers additional light harvesting for the solar cell. In the present work, opto-electrical effects are investigated through quantum efficiency and UV-to-visible spectroscopic measurements. Likewise, a detailed chromaticity analysis, featuring the transmissive and reflective color perception of the device including the mirror, from both sides and in different illumination conditions, is presented and analyzed. Photocurrent density enhancement of up to 21% along with overall device transparency values of up to 31% (4.2% efficiency) is demonstrated for cells showing a colored aesthetic appeal. Finally, a series of simulations emulating the device chromaticity, transparency, and increased photocurrent density as a function of the photoactive layer thickness and the design wavelength of the dielectric mirror are presented. Our simulations and their experimental validation enabled us to establish the design rules that consider the color efficiency/transparency interplay for real applications.

Optical model for simulation and optimization of luminescent down-shifting layers filled with phosphor particles for photovoltaics.

We developed an optical model for simulation and optimization of luminescent down-shifting (LDS) layers for photovoltaics. These layers consist of micron-sized phosphor particles embedded in a polymer binder. The model is based on ray tracing and employs an effective approach to scattering and photoluminescence modelling. Experimental verification of the model shows that the model accurately takes all the structural parameters and material properties of the LDS layers into account, including the layer thickness, phosphor particle volume concentration, and phosphor particle size distribution. Finally, using the verified model, complete organic solar cells on glass substrate covered with the LDS layers are simulated. Simulations reveal that an optimized LDS layer can result in more than 6% larger short-circuit current of the solar cell.

A generic concept to overcome bandgap limitations for designing highly efficient multi-junction photovoltaic cells.

The multi-junction concept is the most relevant approach to overcome the Shockley-Queisser limit for single-junction photovoltaic cells. The record efficiencies of several types of solar technologies are held by series-connected tandem configurations. However, the stringent current-matching criterion presents primarily a material challenge and permanently requires developing and processing novel semiconductors with desired bandgaps and thicknesses. Here we report a generic concept to alleviate this limitation. By integrating series- and parallel-interconnections into a triple-junction configuration, we find significantly relaxed material selection and current-matching constraints. To illustrate the versatile applicability of the proposed triple-junction concept, organic and organic-inorganic hybrid triple-junction solar cells are constructed by printing methods. High fill factors up to 68% without resistive losses are achieved for both organic and hybrid triple-junction devices. Series/parallel triple-junction cells with organic, as well as perovskite-based subcells may become a key technology to further advance the efficiency roadmap of the existing photovoltaic technologies.

High-performance semitransparent perovskite solar cells with solution-processed silver nanowires as top electrodes.

In this work, we report efficient semitransparent perovskite solar cells using solution-processed silver nanowires (AgNWs) as top electrodes. A thin layer of zinc oxide nanoparticles is introduced beneath the AgNWs, which fulfills two essential functionalities: it ensures ohmic contact between the PC60BM and the AgNWs and it serves as a physical foundation that enables the solution-deposition of AgNWs without causing damage to the underlying perovskite. The as-fabricated semitransparent perovskite cells show a high fill factor of 66.8%, Voc = 0.964 V, Jsc = 13.18 mA cm(-2), yielding an overall efficiency of 8.49% which corresponds to 80% of the reference devices with reflective opaque electrodes.

Solution-processed parallel tandem polymer solar cells using silver nanowires as intermediate electrode.

Tandem architecture is the most relevant concept to overcome the efficiency limit of single-junction photovoltaic solar cells. Series-connected tandem polymer solar cells (PSCs) have advanced rapidly during the past decade. In contrast, the development of parallel-connected tandem cells is lagging far behind due to the big challenge in establishing an efficient interlayer with high transparency and high in-plane conductivity. Here, we report all-solution fabrication of parallel tandem PSCs using silver nanowires as intermediate charge collecting electrode. Through a rational interface design, a robust interlayer is established, enabling the efficient extraction and transport of electrons from subcells. The resulting parallel tandem cells exhibit high fill factors of ∼60% and enhanced current densities which are identical to the sum of the current densities of the subcells. These results suggest that solution-processed parallel tandem configuration provides an alternative avenue toward high performance photovoltaic devices.

Fully solution-processing route toward highly transparent polymer solar cells.

We report highly transparent polymer solar cells using metallic silver nanowires (AgNWs) as both the electron- and hole-collecting electrodes. The entire stack of the devices is processed from solution using a doctor blading technique. A thin layer of zinc oxide nanoparticles is introduced between photoactive layer and top AgNW electrode which plays decisive roles in device functionality: it serves as a mechanical foundation which allows the solution-deposition of top AgNWs, and more importantly it facilitates charge carriers extraction due to the better energy level alignment and the formation of ohmic contacts between the active layer/ZnO and ZnO/AgNWs. The resulting semitransparent polymer:fullerene solar cells showed a power conversion efficiency of 2.9%, which is 72% of the efficiency of an opaque reference device. Moreover, an average transmittance of 41% in the wavelength range of 400-800 nm is achieved, which is of particular interest for applications in transparent architectures.

Analytical solution for haze values of aluminium-induced texture (AIT) glass superstrates for a-Si:H solar cells.

Light scattering at randomly textured interfaces is essential to improve the absorption of thin-film silicon solar cells. Aluminium-induced texture (AIT) glass provides suitable scattering for amorphous silicon (a-Si:H) solar cells. The scattering properties of textured surfaces are usually characterised by two properties: the angularly resolved intensity distribution and the haze. However, we find that the commonly used haze equations cannot accurately describe the experimentally observed spectral dependence of the haze of AIT glass. This is particularly the case for surface morphologies with a large rms roughness and small lateral feature sizes. In this paper we present an improved method for haze calculation, based on the power spectral density (PSD) function of the randomly textured surface. To better reproduce the measured haze characteristics, we suggest two improvements: i) inclusion of the average lateral feature size of the textured surface into the haze calculation, and ii) considering the opening angle of the haze measurement. We show that with these two improvements an accurate prediction of the haze of AIT glass is possible. Furthermore, we use the new equation to define optimum morphology parameters for AIT glass to be used for a-Si:H solar cell applications. The autocorrelation length is identified as the critical parameter. For the investigated a-Si:H solar cells, the optimum autocorrelation length is shown to be 320 nm.

Solar power wires based on organic photovoltaic materials.

Organic photovoltaics in a flexible wire format has potential advantages that are described in this paper. A wire format requires long-distance transport of current that can be achieved only with conventional metals, thus eliminating the use of transparent oxide semiconductors. A phase-separated, photovoltaic layer, comprising a conducting polymer and a fullerene derivative, is coated onto a thin metal wire. A second wire, coated with a silver film, serving as the counter electrode, is wrapped around the first wire. Both wires are encased in a transparent polymer cladding. Incident light is focused by the cladding onto to the photovoltaic layer even when it is completely shadowed by the counter electrode. Efficiency values of the wires range from 2.79% to 3.27%.