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Using advanced near UV photoemission spectroscopy PES in constant final state mode CFSYS with very high dynamic range, we investigate the triple cation lead halide perovskite Cs0.05 MA0.17FA0.83 0.95Pb I0.83Br0.17 3 and gain detailed insights into the density of occupied states DOS in the valence band and band gap. A valence band model is established which includes the parabolic valence band edge and an exponentially decaying band tail in a single equation. This allows to precisely determine two valence band maxima VBM at different k vectors in the angle integrated spectra, where the highest one, resulting from the VBM at the R point in the Brillouin zone, is found between 1.50 eV to 1.37 eV relative to the Fermi energy EF. We investigate quantitatively the formation of defect states in the band gap up to EF upon decomposition of the perovskites during sample transfer, storage, and measurements During near UV based PES, the density of defect states saturates at a value that is around four orders of magnitude below the density of states at the valence band edge. However, even short air exposure, or 3h of X ray illumination, increased their density by almost a factor of six and 40, respectively. Upon prolonged storage in vacuum, the formation of a distinct defect peak is observed. Thus, near UV CFSYS with modelling as shown here is demonstrated as a powerful tool to characterize the valence band and quantify defect states in lead halide perovskites

The fullerene C60 is commonly applied as the electron transport layer in high‐efficiency metal halide perovskite solar cells and has been found to limit their open circuit voltage. Through ultra‐sensitive near‐UV photoelectron spectroscopy in constant final state mode (CFSYS), with an unusually high probing depth of 5–10 nm, the perovskite/C60 interface energetics and defect formation is investigated. It is demonstrated how to consistently determine the energy level alignment by CFSYS and avoid misinterpretations by accounting for the measurement‐induced surface photovoltage in photoactive layer stacks. The energetic offset between the perovskite valence band maximum and the C60 HOMO‐edge is directly determined to be 0.55 eV. Furthermore, the voltage enhancement upon the incorporation of a LiF interlayer at the interface can be attributed to originate from a mild dipole effect and probably the presence of fixed charges, both reducing the hole concentration in the vicinity of the perovskite/C60 interface. This yields a field effect passivation, which overcompensates the observed enhanced defect density in the first monolayers of C60.

This work investigates halide segregation in methylammonium-free wide bandgap perovskites by photoluminescence quantum yield (PLQY) and advanced electron microscopy techniques. Our study reveals ho...

Liquid phase crystallized silicon solar cells on glass have recently demonstrated 15.1% efficiency using a heterojunction interdigitated back contact cell architecture and an absorber thickness of 14 $\mu$ m. One of the key enabling developments was a new method to first passivate electron contact fingers with a-Si:H(i) and then locally laser fire them to maintain a low contact resistance. In this work, high resolution, light-beam induced current measurements (LBIC) were used to analyze this approach. Charge collection was observed to have increased from 0.13 ${\text{mAcm}}^{-2}$ to 0.9 ${\text{mAcm}}^{-2}$ under the electron contact which is a sevenfold increase. Using 520, 642, 932, and 1067 nm wavelengths of incident light, external quantum efficiency was mapped in regions including grain boundaries, dislocation defects, shunts, defect-free regions, and laser fired spots. Reduction of charge collection in the laser fired spots was limited to diameters of 50–20 $\mu$ m, depending on whether electrical recombination or optical losses dominated. Effective minority carrier diffusion length under the majority carrier contacts was obtained by fitting of LBIC measurements. It was observed to have improved from 20.5 $\mu$ m to 22.7–40.4 $\mu$ m and up to 89.0 $\mu$ m in the best case. Based on this, wider contact fingers and improved surface passivation at the electron contact is encouraged in the near future to achieve efficiencies $\geq$ 16%.

In this research instrument article, the capabilities and details of a high‐throughput aging system for parallel maximum power point tracking (MPPT) of perovskite solar cells (PSCs), capable of assessing the operational stability of a large number of devices, are presented. The intention is to provide insights into the machine and the development process to engineers who want to create a similar system and eventually make MPPT stability testing of PSCs a standard procedure.

Perovskite/silicon tandem solar cells allow to overcome the power conversion efficiency limit of market-dominating silicon solar cells. So far, various textured tandem devices were presented aiming at improved optical performance, but highest efficiencies were still realized on polished silicon wafer cells enabling superior perovskite layer properties. Here we present perovskite/silicon tandem solar cells with gentle periodic nanotextures which feature various advantages without compromising the material quality of solution-processed perovskite layers. Reflection losses are reduced in comparison to planar tandems and the devices are less sensitive upon deviations from optimum layer thicknesses. The nanotextures also enable excellent perovskite film formation and a greatly increased fabrication yield. The open-circuit voltage improved by about 15 mV due to enhanced electronic properties of the perovskite top cell. In addition, an optically advanced rear reflector with a dielectric buffer layer reduced parasitic absorption at near-infrared wavelengths. Altogether, the improvements enabled a certified power conversion efficiency of 29.80%.

Perovskite-silicon tandem solar cells offer the possibility of overcoming the power conversion efficiency limit of conventional silicon solar cells. Various textured tandem devices have been presented aiming at improved optical performance, but optimizing film growth on surface-textured wafers remains challenging. Here we present perovskite-silicon tandem solar cells with periodic nanotextures that offer various advantages without compromising the material quality of solution-processed perovskite layers. We show a reduction in reflection losses in comparison to planar tandems, with the new devices being less sensitive to deviations from optimum layer thicknesses. The nanotextures also enable a greatly increased fabrication yield from 50% to 95%. Moreover, the open-circuit voltage is improved by 15 mV due to the enhanced optoelectronic properties of the perovskite top cell. Our optically advanced rear reflector with a dielectric buffer layer results in reduced parasitic absorption at near-infrared wavelengths. As a result, we demonstrate a certified power conversion efficiency of 29.80%.

Perovskite–silicon tandem solar cells offer the possibility of overcoming the power conversion efficiency limit of conventional silicon solar cells. Various textured tandem devices have been presented aiming at improved optical performance, but optimizing film growth on surface-textured wafers remains challenging. Here we present perovskite–silicon tandem solar cells with periodic nanotextures that offer various advantages without compromising the material quality of solution-processed perovskite layers. We show a reduction in reflection losses in comparison to planar tandems, with the new devices being less sensitive to deviations from optimum layer thicknesses. The nanotextures also enable a greatly increased fabrication yield from 50% to 95%. Moreover, the open-circuit voltage is improved by 15 mV due to the enhanced optoelectronic properties of the perovskite top cell. Our optically advanced rear reflector with a dielectric buffer layer results in reduced parasitic absorption at near-infrared wavelengths. As a result, we demonstrate a certified power conversion efficiency of 29.80%.

We present results on perovskite/silicon tandem solar cells with almost 30% power conversion efficiency. They comprise sinusoidal nanotextures between top and bottom cells and optically advanced rear reflectors with a dielectric buffer layer.

A quantitative analysis of the thermally induced degradation of various device relevant multi cation hybrid perovskite films is performed using spectroscopic ellipsometry, for temperatures between 80 and 120 C. The studied compositions are a triple cation perovskite Cs0.05 MA0.17FA0.83 0.95Pb Br0.17I0.83 3, a Rb containing variant Rb0.05Cs0.05 MA0.17FA0.83 0.90Pb Br0.17I0.83 3, and a methylammonium free Rb0.05Cs0.10FA0.85PbI3 composition. A very wide combined spectral range of 200 nm to 25 amp; 956;m is covered by combining the data from two separate instruments. The relative changes in organic cation concentrations are quantified from the middle infrared molecular absorption bands, leveraging the use of point by point fitting for increased sensitivity. Additionally, the formation of PbI2 and non perovskite amp; 948; CsPbI3 phases is evidenced from Bruggemann effective medium fits to the visible and ultraviolet complex refractive indices. Methylammonium is almost completely depleted from the relevant compositions within 100 to 285 min of thermal annealing. The MA free perovskite degrades faster at intermediate temperatures, which is attributed to phase instability due to the formation of amp; 948; CsPbI3 in addition to PbI2

Combining the emerging perovskite solar cell technology with existing silicon approaches in a tandem cell design offers the possibility for new low-cost high-performance devices. In this study, the potential of liquid phase crystallized silicon (LPC-Si) solar cells as a bottom cell in an all-thin-film tandem device is investigated. By optimizing the current output of a four terminal tandem using optical simulations and state-of-the-art electrical properties of the top and bottom cells, we show that an efficiency of 23.3 $\%$ can be reached, where 7.2 $\%$ are attributed to the LPC-Si bottom cell. Including the potential of future developments of both sub cells, efficiencies of over 28 $\%$ are estimated. Electrical and optical measurements of the bottom cell are performed by attaching a perovskite and a cutoff filter to the front side of the interdigitated back contacted LPC-Si cells. The measurements using a cutoff filter show a high impact of the filtered incident light spectrum on the open circuit voltage of the LPC-Si cell. A comparison of the simulated and measured absorptance shows that especially the optical properties of the transparent conductive oxides and recombination losses in the LPC-Si cause high current losses. Combining the measured data of the filtered LPC-Si cells and the semitransparent perovskite cells, yields a realistic estimation for the efficiency of a state-of-the-art four-terminal tandem device of 19.3 $\%$ .

Halide perovskites are a strong candidate for the next generation of photovoltaics. Chemical doping of halide perovskites is an established strategy to preparethe highest efficiency andmost stable perovskite-based solar cells. In this study, we unveil the doping mechanism of halide perovskites using a series of alkaline earth metals. We find that low doping levels enable the incorporation of the dopant within the perovskite lattice, whereas high doping concentrations induce surface segregation. The threshold from low to high doping regime correlates to the size of the doping element. We show that the low doping regime results in a more n-typematerial, while the high doping regime induces a less n-type doping character. Our work provides a comprehensive picture of the unique doping mechanism of halide perovskites, which differs fromclassical semiconductors. We proved the effectiveness of the low doping regime for the first time, demonstrating highly efficient methylammonium lead iodide based solar cells in both n-i-p and p-i-n architectures.

Formamidinium iodide FAI based perovskite absorbers have been shown to be ideal candidates for highly efficient and operationally stable perovskite solar cells PSC . A major challenge for formamidinium lead iodide FAPbI3 is to suppress the phase transition from the photoactive black phase into yellow nonperovskite amp; 948; phase. Several approaches to stabilize the black phase have been developed for solution based perovskites, whereas so far, vacuum deposited FAPbI3 has rarely been reported. This study demonstrates the preparation of FAPbI3 by co evaporation and discusses the influence of the subjacent hole transporting layer HTL on its phase stability. By using FAI excess in the evaporation process in combination with phosphonic acids groups from the HTL, the black perovskite phase is stabilized at room temperature. Further addition of 32 59 methylammonium iodide MAI during the co evaporation process leads to good absorption properties and high PSC efficiencies of 20.4 . In addition, excellent stability is achieved for optimized MAI to FAI ratios, maintaining 100 of the initial PSC performance after 1000 h under constant operation. This highly stable perovskite composition enables the first monolithic fully textured perovskite silicon tandem solar cells with co evaporated perovskite absorbers. Due to the conformally covered pyramid texture, these tandem cells show minimal reflection losses and reach an efficiency of 24.6

The operation of halide perovskite optoelectronic devices, including solar cells and LEDs, is strongly influenced by the mobility of ions comprising the crystal structure. This peculiarity is particularly true when considering the long-term stability of devices. A detailed understanding of the ion migration-driven degradation pathways is critical to design effective stabilization strategies. Nonetheless, despite substantial research in this first decade of perovskite photovoltaics, the long-term effects of ion migration remain elusive due to the complex chemistry of lead halide perovskites. By linking materials chemistry to device optoelectronics, this study highlights that electrical bias-induced perovskite amorphization and phase segregation is a crucial degradation mechanism in planar mixed halide perovskite solar cells. Depending on the biasing potential and the injected charge, halide segregation occurs, forming crystalline iodide-rich domains, which govern light emission and participate in light absorption and photocurrent generation. Additionally, the loss of crystallinity limits charge collection efficiency and eventually degrades the device performance.

Doped spiro-OMeTAD at present is the most commonly used hole transport material (HTM) in n-i-p-type perovskite solar cells, enabling high efficiencies around 22%. However, the required dopants were shown to induce nonradiative recombination of charge carriers and foster degradation of the solar cell. Here, in a novel approach, highly conductive and inexpensive water-free poly(3,4-ethylenedioxythiophene) (PEDOT) is used to replace these dopants. The resulting spiro-OMeTAD/PEDOT (SpiDOT) mixed films achieve higher lateral conductivities than layers of doped spiro-OMeTAD. Furthermore, combined transient and steady-state photoluminescence studies reveal a passivating effect of PEDOT, suppressing nonradiative recombination losses at the perovskite/HTM interface. This enables excellent quasi-Fermi level splitting values of up to 1.24 eV in perovskite/SpiDOT layer stacks and high open-circuit voltages (V-OC) up to 1.19 V in complete solar cells. Increasing the amount of dopant-free spiro-OMeTAD in SpiDOT layers is shown to enhance hole extraction and thereby improves the fill factor in solar cells. As a consequence, stabilized efficiencies up to 18.7% are realized, exceeding cells with doped spiro-OMeTAD as a HTM in this study. Moreover, to the best of our knowledge, these results mark the lowest nonradiative recombination loss in the V-OC (140 mV with respect to the Shockley-Queisser limit) and highest efficiency reported so far for perovskite solar cells using PEDOT as a HTM.

Summary Monolithic [Cs0.05(MA0.17FA0.83)0.95]Pb(I0.83Br0.17)3/Cu(In,Ga)Se2 (perovskite/CIGS) tandem solar cells promise high performance and can be processed on flexible substrates, enabling cost-efficient and ultra-lightweight space photovoltaics with power-to-weight and power-to-cost ratios surpassing those of state-of-the-art III-V semiconductor-based multijunctions. However, to become a viable space technology, the full tandem stack must withstand the harsh radiation environments in space. Here, we design tailored operando and ex situ measurements to show that perovskite/CIGS cells retain over 85% of their initial efficiency even after 68 MeV proton irradiation at a dose of 2 × 1012 p+/cm2. We use photoluminescence microscopy to show that the local quasi-Fermi-level splitting of the perovskite top cell is unaffected. We identify that the efficiency losses arise primarily from increased recombination in the CIGS bottom cell and the nickel-oxide-based recombination contact. These results are corroborated by measurements of monolithic perovskite/silicon-heterojunction cells, which severely degrade to 1% of their initial efficiency due to radiation-induced recombination centers in silicon., Graphical Abstract, Highlights • Halide perovskite sub-cells exhibit strong proton irradiation resiliency • Novel operando characterization distinguishes degradation of individual sub-cells • Perovskite/CIGS tandem solar cells retain 85% of their initial efficiency after irradiation • Perovskite/SHJ tandem solar cells degrade to 1% of their initial efficiency after irradiation, Context & Scale Monolithic perovskite/silicon and perovskite/CIGS tandem solar cells could facilitate large-scale decarbonization of the power sector, provided their long-term stability is proven. In this work, we test the stability of both technologies under high-energy proton irradiation. While this mimics the radiation environment in space, our versatile operando and ex situ methodology is also suitable for studying the long-term stability of multijunction solar cells for terrestrial applications. We find that perovskite/silicon tandem solar cells are unsuitable for space, whereas perovskite/CIGS tandems are radiation-hard, promising cheap, flexible, and ultra-lightweight space photovoltaics. Both the growing demand for smaller, cheaper satellites and the privatization of space exploration are revolutionizing space economics, providing an ideal niche for the commercialization of this new technology until the levelized cost-of-electricity can compete with current terrestrial photovoltaics., We propose and test monolithic perovskite/CIGS tandem solar cells for readily stowable, ultra-lightweight space photovoltaics. We design operando and ex situ measurements to show that perovskite/CIGS tandem solar cells retain over 85% of their initial power-conversion efficiency after high-energy proton irradiation. While the perovskite sub-cell is unaffected after this bombardment, we identify increased non-radiative recombination in the CIGS bottom cell and nickel-oxide-based recombination layer. By contrast, monolithic perovskite/silicon-heterojunction cells degrade to 1% of their initial efficiency due to radiation-induced defects in silicon.

Perovskite based tandem solar cells can increase the power conversion efficiency PCE of conventional single junction photovoltaic devices. Here, we present monolithic perovskite CIGSe tandem solar cells with a perovskite top cell fabricated directly on an as grown, rough CIGSe bottom cell. To prevent potential shunting due to the rough CIGSe surface, a thin NiOx layer is conformally deposited via atomic layer deposition on the front contact of the CIGSe bottom cell. The performance is further improved by an additional layer of the polymer PTAA at the NiOx perovskite interface. This hole transport bilayer enables a 21.6 stabilized PCE of the tandem device at amp; 8764;0.8 cm2 active area. We use TEM EDX measurements to investigate the deposition uniformity and conformality of the NiOx and PTAA layers. By absolute photoluminescence measurements, the contribution of the individual subcells to the tandem VOC is determined, revealing that further fine tuning of the recombination layers might improve the tandem VOC. Finally, on the basis of the obtained results, we give guidelines to improve monolithic perovskite CIGSe tandems toward predicted PCE estimates above 30

Metal halide perovskites show great promise to enable highly efficient and low cost tandem solar cells when being combined with silicon. Here, we combine rear junction silicon heterojunction bottom cells with p-i-n perovskite top cells into highly efficient monolithic tandem solar cells with a certified power conversion efficiency (PCE) of 25.0%. Further improvements are reached by reducing the current mismatch of the certified device. The top contact and perovskite thickness optimization allowed increasing the J SC above 19.5 mA cm -2, enabling a remarkable tandem PCE of 26.0%, however with a slightly limited fill factor (FF). To test the dependency of the FF on the current mismatch between the sub-cells, the tandems' J-V curves are measured under various illumination spectra. Interestingly, the reduced J SC in unmatched conditions is partially compensated by an enhancement of the FF. This finding is confirmed by electrical simulations based on input parameters from reference single junction devices. The simulations reveal that especially the FF in the experiment is below the expected value and show that with improved design we could reach 29% PCE for our monolithic perovskite/silicon tandem device and 31% PCE if record perovskite and silicon cell single junctions could be combined in tandem solar cells.

The incorporation of even small amounts of strontium (Sr) into lead-base hybrid quadruple cation perovskite solar cells results in a systematic increase of the open circuit voltage (V-oc) in pin-type perovskite solar cells. We demonstrate via absolute and transient photoluminescence (PL) experiments how the incorporation of Sr significantly reduces the non-radiative recombination losses in the neat perovskite layer. We show that Sr segregates at the perovskite surface, where it induces important changes of morphology and energetics. Notably, the Sr-enriched surface exhibits a wider band gap and a more n-type character, accompanied with significantly stronger surface band bending. As a result, we observe a significant increase of the quasi-Fermi level splitting in the neat perovskite by reduced surface recombination and more importantly, a strong reduction of losses attributed to non-radiative recombination at the interface to the C-60 electron-transporting layer. The resulting solar cells exhibited a V-oc of 1.18 V, which could be further improved to nearly 1.23 V through addition of a thin polymer interlayer, reducing the non-radiative voltage loss to only 110 meV. Our work shows that simply adding a small amount of Sr to the precursor solutions induces a beneficial surface modification in the perovskite, without requiring any post treatment, resulting in high efficiency solar cells with power conversion efficiency (PCE) up to 20.3%. Our results demonstrate very high V-oc values and efficiencies in Sr-containing quadruple cation perovskite pin-type solar cells and highlight the imperative importance of addressing and minimizing the recombination losses at the interface between perovskite and charge transporting layer.

Liquid phase crystallization of silicon (LPC-Si) offers great potential for high-quality Si films and a cost effective fabrication technique for thin crystalline silicon solar cells on glass. In this work, we report on the progress on LPC-silicon at HZB in the past years. Beginning with a brief description of the fabrication process, we summarize the work on the different contact systems developed for these absorbers before focusing on the interdigitated back contact architecture on which the highest efficiencies were reported. State-of-the art cells form the basis for a detailed discussion of the status of this technology. We investigate the current loss mechanisms and explore the potential for further improvement. Finally, based on this comprehensive quality assessment, we develop a roadmap to increase the cell efficiencies to wafer-equivalent values.

Laser based patterning for monolithic serial interconnection of metal halide perovskite MHP solar cells is a key process for industrial manufacturing of large scale MHP solar panels. It requires reliable patterning process parameters to achieve low interconnection losses and, thus, high efficiencies. Here, P2 laser patterning of the perovskite layer was obtained by laser ablation using conventional nanosecond laser pulses at systematically varied laser fluences. The correlation of the laser impact to the morphology, composition, and electrical functionality was analyzed in detail by several surface analytical techniques. The occurrence of laser induced periodic surface structures and microdroplets at the bottom of the trenches indicates that material removal via stress assisted ablation is strongly influenced by thermal processes. The formation of PbI 2 containing residuals was evidenced, possibly causing contact resistance losses through the P2 interconnect. These results contribute to the identification of loss factors in laser based serial interconnection of perovskite solar cells and to further process optimization for upscaling to industrial module sizes

Liquid phase crystallization of silicon (LPC-Si) on glass is a promising method to produce high quality multi-crystalline Si films with macroscopic grains. In this study, we report on recent improvements of our interdigitated back-contact silicon heterojunction contact system (IBC-SHJ), which enabled open circuit voltages as high as 661 mV and efficiencies up to 14.2% using a 13 µm thin n-type LPC-Si absorbers on glass. The influence of the BSF width on the cell performance is investigated both experimentally and numerically. We combine 1D optical simulations using GenPro4 and 2D electrical simulations using Sentaurus™ TCAD to determine the optical and electrical loss mechanisms in order to estimate the potential of our current LPC-Si absorbers. The simulations reveal an effective minority carrier diffusion length of 26 µm and further demonstrate that a doping concentration of 4 × 10 16 cm −3 and a back surface field width of 60 µm are optimum values to further increase cell efficiencies.

Efficient light management in monolithic perovskite/silicon tandem solar cells is one of the prerequisites for achieving high power conversion efficiencies (PCEs). Textured silicon wafers can be utilized for light management, however, this is typically not compatible with perovskite solution processing. Here, we instead employ a textured light management (LM) foil on the front-side of a tandem solar cell processed on a wafer with a planar front-side and textured back-side. This way the PCE of monolithic, 2-terminal perovskite/silicon-heterojunction tandem solar cells is significantly improved from 23.4% to 25.5%. Furthermore, we validate an advanced numerical model for our fabricated device and use it to optically optimize a number of device designs with textures at different interfaces with respect to the PCE and energy yield. These simulations predict a slightly lower optimal bandgap of the perovskite top cell in a textured device as compared to a flat one and demonstrate strong interdependency between the bandgap and the texture position in the monolithic stack. We estimate the PCE potential for the best performing both-side textured device to be 32.5% for a perovskite bandgap of 1.66 eV. Furthermore, the results show that under perpendicular illumination conditions, for optimized designs, the LM foil on top of the cell performs only slightly better than a flat anti-reflective coating. However, under diffuse illumination, the benefits of the LM foil are much greater. Finally, we calculate the energy yield for the different device designs, based on true weather data for three different locations throughout the year, taking direct as well as diffuse illumination fully into account. The results further confirm the benefits of front-side texture, even more for BIPV applications. Overall, devices built on a both-side textured silicon wafer perform best. However, we show that devices with textured LM foils on the cell's front-side are a highly efficient alternative.

Liquid-phase crystallization (LPC) of thin silicon layers on glass substrates is a technique to fabricate solar cells with low energy and material consumption and open-circuit voltages comparable to multicrystalline silicon wafer cells. We studied the impact of different passivation layers deposited with plasma-enhanced chemical vapor deposition (PECVD) on the cell quality. Silicon nitride (SiNx) and ultrathin silicon oxide (SiO x ) layers with varying thicknesses were used. In addition, we plasma-treated the SiN x surface to form a thin silicon oxynitride (SiO x N y ) passivation layer. Plasma oxidation is an attractive alternative to PECVD, since thicknesses of ultrathin layers can be controlled easier as compared with PECVD. We found that the cell performance is influenced by the passivation layer. Particularly, cells on the 9 nm PECVD SiO x passivation layer are worse than cells on the 11 nm SiO x N y layer. We modeled cell parameters employing ASPIN3 to estimate effective diffusion lengths. Using transmission electron microscopy as well as electron energy loss spectroscopy, we studied the effect of the plasma treatment on the morphology and elemental distribution at the interface between passivation layer and LPC-Si absorber. Our best interdigitated back contacted solar cell with an efficiency >14% is based on the SiO x N y layer.

Liquid phase crystallization using line-shaped energy sources such as CW-diode lasers or electron beams has proven to form mc-Si layers on borosilicate or borosilicate/aluminosilicate glass that exhibit wafer equivalent grain sizes and electronic quality. In this work, we characterize the impact of the employed dielectric interlayer stack sandwiched between glass and absorber on the electronic quality. For this purpose, we investigate a large variety of test cell results achieved in the past on different interlayer stacks composed of silicon oxide, silicon nitride as well as silicon oxynitride deposited by means of plasma enhanced chemical vapour deposition or plasma oxidation and employ i(v), SunsVoc, quantum efficiency measurements, and photoluminescence imaging to assess the electronic properties of the crystallized absorbers. The results are compared with state-of the art interdigitated back-contact cells and literature values. Based on these findings, we conclude that at the present state of interlayer , the bulk quality imposes the limits in cell efficiency and investigates potential approaches to increase the bulk quality of LPC-Si absorbers.

We report on two differentapproaches to fabricateinterdigitated back contact silicon heterojunction solarcells without using indium tin oxide (ITO). The standard ITO/Ag backend is either modified by replacing ITO with aluminum-doped zinc oxide (AZO) or completely replaced by a sole aluminum (Al) layer. The very transparent AZO enhances the optical properties at the rear side resulting in an increase in short-circuit current density.The efficiency of the AZO cells remains on the level of the ITO ones, as the fillfactor drops slightly. On the contrary, the contact resistivity of annealed Al, in comparison to ITO and AZO, to the emitter and BSF layers is much lower, thus the fill factor is increased. Despite lower open circuit voltages,cells with Al achieve efficiencies of up 22 %, a gain of 0.5 %abs compared to the ITO reference.

Inorganic-organic perovskites like methylammonium-lead-iodide have proven to be an effective class of 17 materials for fabricating efficient solar cells. To improve their performance, light management techniques using textured surfaces, similar to those used in established solar cell technologies, should be considered. Here, we apply a light management foil created by UV nanoimprint lithography on the glass side of an inverted (p-i-n) perovskite solar cell with 16.3% efficiency. The obtained 1 mA cm(-2) increase in the short-circuit current density translates to a relative improvement in cell performance of 5%, which results in a power conversion efficiency of 17.1%. Optical 3D simulations based on experimentally obtained parameters were used to support the experimental findings. A good match between the simulated and experimental data was obtained, validating the model. Optical simulations reveal that the main improvement in device performance is due to a reduction in total reflection and that relative improvement in the short-circuit current density of up to 10% is possible for large-area devices. Therefore, our results present the potential of light management foils for improving the device performance of perovskite solar cells and pave the way for further use of optical simulations in the field of perovskite solar cells.

For methylammonium lead iodide perovskite solar cells prepared by co-evaporation, power conversion efficiencies of over 20% have been already demonstrated, however, so far, only in n-i-p configuration. Currently, the overall major challenges are the complex evaporation characteristics of organic precursors that strongly depend on the underlying charge selective contacts and the insufficient reproducibility of the co-evaporation process. To ensure a reliable co-evaporation process, it is important to identify the impact of different parameters in order to develop a more detailed understanding. In this work, we study the influence of the substrate temperature, underlying hole-transport layer (polymer PTAA versus self-assembling monolayer molecule MeO-2PACz), and perovskite precursor ratio on the morphology, composition, and performance of co-evaporated p-i-n perovskite solar cells. We first analyze the evaporation of pure precursor materials and show that the adhesion of methylammonium iodide (MAI) is significantly reduced with increased substrate temperature, while it remains almost unaffected for lead iodide (PbI

Halide perovskites are a strong candidate for the next generation of photovoltaics. Chemical doping of halide perovskites is an established strategy to prepare the highest efficiency and most stable perovskite-based solar cells. In this study, we unveil the doping mechanism of halide perovskites using a series of alkaline earth metals. We find that low doping levels enable the incorporation of the dopant within the perovskite lattice, whereas high doping concentrations induce surface segregation. The threshold from low to high doping regime correlates to the size of the doping element. We show that the low doping regime results in a more n-type material, while the high doping regime induces a less n-type doping character. Our work provides a comprehensive picture of the unique doping mechanism of halide perovskites, which differs from classical semiconductors. We proved the effectiveness of the low doping regime for the first time, demonstrating highly efficient methylammonium lead iodide based solar cells in both n-i-p and p-i-n architectures.

Efficiency from hole-selective contacts Perovskite/silicon tandem solar cells must stabilize a perovskite material with a wide bandgap and also maintain efficient charge carrier transport. Al-Ashouri et al. stabilized a perovskite with a 1.68–electron volt bandgap with a self-assembled monolayer that acted as an efficient hole-selective contact that minimizes nonradiative carrier recombination. In air without encapsulation, a tandem silicon cell retained 95% of its initial power conversion efficiency of 29% after 300 hours of operation. Science , this issue p. 1300

The operation of halide perovskite optoelectronic devices, including solar cells and LEDs, is strongly influenced by the mobility of ions comprising the crystal structure. This peculiarity is particularly true when considering the long‐term stability of devices. A detailed understanding of the ion migration‐driven degradation pathways is critical to design effective stabilization strategies. Nonetheless, despite substantial research in this first decade of perovskite photovoltaics, the long‐term effects of ion migration remain elusive due to the complex chemistry of lead halide perovskites. By linking materials chemistry to device optoelectronics, this study highlights that electrical bias‐induced perovskite amorphization and phase segregation is a crucial degradation mechanism in planar mixed halide perovskite solar cells. Depending on the biasing potential and the injected charge, halide segregation occurs, forming crystalline iodide‐rich domains, which govern light emission and participate in light absorption and photocurrent generation. Additionally, the loss of crystallinity limits charge collection efficiency and eventually degrades the device performance.

—Liquid phase crystallized silicon (LPC-Si) solar cells on glass have demonstrated 14.2 % efficiency using a heterojunction interdigitated back contact cell architecture and an absorber thickness of 13 µm. However, losses are incurred in charge collection under the majority carrier contact regions even after reducing their width to 60 −120 µm. Recently, we developed a new method to first passivate these contact fingers with a-Si:H(i) and then locally laser-fire them to maintain a low contact resistance. High resolution light beam induced current measurements were used to analyze these developments. Without a-Si:H(i), an effective minority carrier diffusion length around 19 µm under the majority carrier contacts lead to only 0.13 mA cm−2 being collected there. With the new method, the diffusion length was improved to 36 µm and up to 113.6 µm in the best case. The reduction of passivation in the laser-fired spots was limited to a diameter of 55 µm. Over-all, charge collection increased by 0.8 mA cm−2 under the electron contact. Spatial mapping of charge collection creates a clear outlook to achieve 15 % efficiency even with the current material quality by reducing the laser firing spot size and implementing the new approach on cells with larger and more uniform grains.

In this paper, we report on the current status of absorber attributes in Liquid Phase Crystallized Silicon (LPC-Si) cells. To this end, an absorber doping series (ND = 2·1016/cm³ to 7·1017/cm³) and an absorber thickness variation (14 and 33 µm) are evaluated. Best cells from the batches for these series showed open circuit voltages up to 640 mV and fill factors above 70%. It is observed that for state-of-the-art cells, thicknesses over 15 µm are not beneficial due to limited diffusion lengths. Lower absorber doping concentrations tend to yield longer intra-grain diffusion lengths (Ldiff) and better passivated grain boundaries, which may be due to lower impurity precipitation. The longer Ldiff leads to higher short circuit current densities which over-compensate a decrease in open circuit voltage and fill factor with regards to efficiency. Both front and rear surfaces are sufficiently passivated and at the current status the bulk lifetime has most potential for improvement.

We develop a method to quantify the local minority carrier diffusion lengths in interdigitated back-contact solar cells having a 10- µ m-thick liquid-phase crystallized (LPC) Si absorber by light-beam induced current (LBIC) measurements. The method is verified by 2-D simulations of the LBIC signals using ASPIN3. The effective minority carrier diffusion lengths determined this way range between 33 and 44 µ m inside a grain, which proves that advanced cell concepts like an interdigitated back contact (IBC) system are well suited for the LPC absorbers. Furthermore, the method has the potential to help improve the optimization of contact system geometries, and it may be used to understand the influences of different grain orientations and improve the LPC-Si absorber fabrication process.

A major limitation in current liquid-phase crystallized (LPC) silicon thin-film record solar cells is optical losses caused by their planar glass–silicon interface. In this study, silicon is grown on nanoimprinted periodically, as well as randomly textured glass substrates, and successfully implemented into state-of-the-art LPC silicon thin-film solar cells. Compared with an optimized planar reference device, both textures enhance absorption of light. Interlayer and process optimization allowed achieving a material quality comparable with the planar reference device. On the random texture, an open-circuit voltage above 630 mV was obtained, as well as an external quantum efficiency exceeding the planar reference device by +3 mA/cm2.

The passivation quality at the interface between liquid-phase crystallized silicon (LPC-Si) and a dielectric interlayer (IL) was investigated in terms of the defect state density at the IL/LPC-Si interface (Dit) as well as the effective fixed charge density in the IL (QIL,eff). Both parameters were obtained via high-frequency capacitance–voltage measurements on developed metal–insulator–semiconductor structures based on a molybdenum layer sandwiched between the IL and the glass substrate. Dit and QIL,eff were correlated to the open circuit voltage (Voc) and the integrated external quantum efficiency (Jsc,EQE) obtained on corresponding solar cell structures as well as to Voc and Jsc,EQE results based on two-dimensional simulations. We found that Dit was reduced by one order of magnitude using a hydrogen plasma treatment (HPT) at 400 °C. Irrespectively of the HPT, QIL,eff was > 1012 cm−2. We suggest that field-effect passivation dominates chemical passivation at the IL/n-type LPC-Si interface. We attribute the significant enhancement of Voc and Jsc,EQE observed after HPT on n-type LPC-Si solar cells mainly to improvements of the passivation quality in the n-type LPC-Si bulk rather than at the IL/n-type LPC-Si interface. For p-type absorbers, the HPT did not improve Voc and Jsc,EQE significantly. We propose that this is because of an insufficient passivation of bulk defects by positively charged hydrogen, which dominates in p-type silicon, in combination with an insufficient interface passivation. Copyright © 2016 John Wiley & Sons, Ltd.

Amorphous/microcrystalline/crystalline silicon (a-Si:H/μc-Si:H/c-Si) triple junction solar cells have been developed to directly split water, for which operating voltages (Voc) >1.5 V (depending on the catalysts) are needed. These cells are an inexpensive alternative to high efficiency, high voltage multi junction solar cells based on scarce elements like III-V semiconductors. To obtain a dense μc-Si:H middle cell with high Voc, we investigated a second acid-based polishing step to systematically smoothen the sharp V-shaped valleys present after standard KOH pyramid texturing. This way, we reduced defective regions in the 2 – 3 μm thick μc-Si:H middle and the 250 – 300 nm thick a-Si:H top cell. Quantitatively analyzing the surfaces by atomic force microscopy, we found that a reduction from 49° to 25° in the maximum of the angle distribution of the surface allowed an increase in Voc of >130 mV and an increase in fill factor (FF) from ∼50% to >70%. By further optimizing the nanocrystalline silicon oxide (nc-SiOx:H) intermediate reflector layer placed between bottom and middle cell, the nc-SiOx:H top cell p-layer as well as middle cell thickness, we could increase the solar to electricity conversion efficiency to 12.7%. Very promising first results are presented by utilizing the triple junction cell for stand-alone water splitting device in alkaline electrolysis as demonstrated by using a standard 3-electrode setup.

In recent years, thin-film silicon solar cells on glass prepared by liquid-phase crystallization have made progress towards high efficiency solar cells. Current record cells reach wafer-equivalent material quality and morphology using thin-film technologies. However, short-circuit current densities and hence, efficiencies, are still limited. The reflection at the interface between glass superstrate and silicon absorber layer has been identified as one major loss mechanism. These optical losses can be reduced by nanostructuring of the interface. It is important, however, that this nanostructured interface does not lead to a deterioration of silicon material quality simultaneously. Recently, we introduced SMooth Anti-Reflective Three-dimensional (SMART) textures, which consist of temperature-stable SiO x sol-gel nanostructures and a smoothing layer of spin-coated TiO x . These SMART textures on glass superstrates exhibit a smooth interface morphology and hence allow growing high-quality silicon absorber layers by liquid phase crystallization. Here, we investigate the optical properties of the SMART textures with and without an additional SiN x layer in experiment and by 1-dimensional optical simulations. It is shown that both, the SMART textures with and without additional SiN x layer, can outperform the optimized planar interlayer system of current record solar cell devices. Very low mean reflectance values of 11.2% are found in the wavelength regime from 400 nm to 600 nm for an optimized texture consisting of a 50 nm thick SMART texture with additional 15 nm SiN x layer.