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Wide bandgap halide perovskite materials show promising potential to pair with silicon bottom cells. To date, most efficient wide bandgap perovskites layers are fabricated by spin coating, which is difficult to scale up. Here, we report on slot die coating for an efficient, 1.68 eV wide bandgap triple halide 3halide perovskite absorber, Cs0.22FA0.78 Pb I0.85Br0.15 3 5 mol MAPbCl3. A suitable solvent system is designed specifically for the slot die coating technique. We demonstrate that our fabrication route is suitable for tandem solar cells without phase segregation. The slot die coated wet halide perovskite is dried by a nitrogen N2 knife with high reproducibility and avoiding antisolvents. We explore varying annealing conditions and identify parameters allowing crystallization of the perovskite film into large grains reducing charge collection losses and enabling higher current density. At 150 C, an optimized trade off between crystallization and the PbI2 aggregates on the film s top surface is found. Thus, we improve the cell stability and performance of both single junction cells and tandems. Combining the 3halide top cells with a 120 amp; 956;m thin saw damage etched commercial Czochralski industrial wafer, a 2 terminal monolithic tandem solar cell with a PCE of 25.2 on a 1 cm2 active area is demonstrated with fully scalable processes

The wettability issue associated with the Me-4PACz hole-selective monolayer is solved by the introduction of the second component to the precursor solution. This results in a similar performance while simultaneously significantly improving the yield of the devices.

Metal halide perovskites have attracted tremendous attention due to their excellent electronic properties. Recent advancements in device performance and stability of perovskite solar cells (PSCs) have been achieved with the application of self-assembled monolayers (SAMs), serving as stand-alone hole transport layers in the p-i-n architecture. Specifically, phosphonic acid SAMs, directly functionalizing indium-tin oxide (ITO), are presently adopted for highly efficient devices. Despite their successes, so far, little is known about the surface coverage of SAMs on ITO used in PSCs application, which can affect the device performance, as non-covered areas can result in shunting or low open-circuit voltage. In this study, we investigate the surface coverage of SAMs on ITO and observe that the SAM of MeO-2PACz ([2-(3,6-dimethoxy-9H-carbazol-9-yl)ethyl]phosphonic acid) inhomogeneously covers the ITO substrate. Instead, when adopting an intermediate layer of NiO between ITO and the SAM, the homogeneity, and hence the surface coverage of the SAM, improve. In this work, NiO is processed by plasma-assisted atomic layer deposition (ALD) with Ni(MeCp)2 as the precursor and O2 plasma as the co-reactant. Specifically, the presence of ALD NiO leads to a homogeneous distribution of SAM molecules on the metal oxide area, accompanied by a high shunt resistance in the devices with respect to those with SAM directly processed on ITO. At the same time, the SAM is key to the improvement of the open-circuit voltage of NiO + MeO-2PACz devices compared to those with NiO alone. Thus, the combination of NiO and SAM results in a narrower distribution of device performance reaching a more than 20% efficient champion device. The enhancement of SAM coverage in the presence of NiO is corroborated by several characterization techniques including advanced imaging by transmission electron microscopy (TEM), elemental composition quantification by Rutherford backscattering spectrometry (RBS), and conductive atomic force microscopy (c-AFM) mapping. We believe this finding will further promote the usage of phosphonic acid based SAM molecules in perovskite PV.

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.

Light management strategies can increase the efficiency of perovskite single-junction and tandem solar cells. In this study, we present perovskite solar cells deposited on different shallow nanotex...

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 demonstrate a monolithic perovskite CIGS tandem solar cell with a certified power conversion efficiency PCE of 24.2 . The tandem solar cell still exhibits photocurrent mismatch between the subcells; thus optical simulations are used to determine the optimal device stack. Results reveal a high optical potential with the optimized device reaching a short circuit current density of 19.9 mA cm 2 and 32 PCE based on semiempirical material properties. To evaluate its energy yield, we first determine the CIGS temperature coefficient, which is at amp; 8722;0.38 K 1 notably higher than the one from the perovskite subcell amp; 8722;0.22 K 1 , favoring perovskite in the field operation at elevated cell temperatures. Both single junction cells, however, are significantly outperformed by the combined tandem device. The enhancement in energy output is more than 50 in the case of CIGS single junction device. The results demonstrate the high potential of perovskite CIGS tandem solar cells, for which we describe optical guidelines toward 30 PCE

et al., Large datasets are now ubiquitous as technology enables higher-throughput experiments, but rarely can a research field truly benefit from the research data generated due to inconsistent formatting, undocumented storage or improper dissemination. Here we extract all the meaningful device data from peer-reviewed papers on metal-halide perovskite solar cells published so far and make them available in a database. We collect data from over 42,400 photovoltaic devices with up to 100 parameters per device. We then develop open-source and accessible procedures to analyse the data, providing examples of insights that can be gleaned from the analysis of a large dataset. The database, graphics and analysis tools are made available to the community and will continue to evolve as an open-source initiative. This approach of extensively capturing the progress of an entire field, including sorting, interactive exploration and graphical representation of the data, will be applicable to many fields in materials science, engineering and biosciences., Open access funding provided by Helmholtz-Zentrum Berlin für Materialien und Energie GmbH., The core funding of the project has been received from the European Union’s Horizon 2020 research and innovation programme under grant agreement no. 787289. We acknowledge the following sources for individual funding. Cambridge India Ramanujan Scholarship, China Scholarship Council, Deutscher Akademischer Austauschdienst (DAAD), EPSRC (grant no. EP/S009213/1), European Union’s Horizon 2020 research and innovation programme (grant no. 764787, EU Project ‘MAESTRO’), (grant no. 756962, ERC Project ‘HYPERION’), (grant no. 764047, EU Project ‘ESPResSo’ and grant no. 850937), GCRF/EPSRC SUNRISE (EP/P032591/1), German Federal Ministry for Education and Research (BMBF), HyPerFORME, NanoMatFutur (grant no. 03XP0091). PEROSEED (ZT-0024), Helmholtz Energy Materials Foundry, The Helmholtz Innovation Laboratory HySPRINT. BMBF (grant nos. 03SF0540, 03SF0557A), HyPerCells graduate school, Helmholtz Association, Helmholtz International Research School (HI-SCORE), the Erasmus programme (CDT-PV, grant no. EP/L01551X/1), the European Union’s Horizon 2020 research and innovation programme (Marie Skłodowska-Curie grant agreement nos. 841386, 795079 and 840751), Royal Society University Research Fellowship (grant no. UF150033). SNaPSHoTs (BMBF), SPARC II, German Research Foundation (DFG, grant no. SPP2196), The National Natural Science Foundation of China (grant no. 51872014), the Recruitment Programme of Global Experts, Fundamental Research Funds for the Central Universities and the ‘111’ project (grant no. B17002), the US Department of Energy’s Office of Energy Efficiency and Renewable Energy under Solar Energy Technologies Office (SETO) agreement no. DE-EE0008551, the Colombia Scientific Programme in the framework of the call Ecosistema Cientifíco (Contract no. FP44842-218-2018), the committee for the development of research (CODI) of the Universidad de Antioquia (grant no. 2017-16000), Spanish MINECO (Severo Ochoa programme, grant no. SEV‐2015‐0522), the Swedish research council (VR, grant no. 2019-05591) and the Swedish Energy Agency (grant no. 2020-005194).

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

This work focuses on 2D device simulation for perovskite/tandem solar cells, aiming to reproduce the experimental current-voltage curves and to explore further steps for efficiency improvements. The results demonstrate that a reasonable J-V curve can be obtained when the indium tin oxide (ITO) layer that interconnects both subcells is treated as either a semiconductor or conductor. In both cases, band to band tunneling and/or additional built-in voltage governed by proper work functions of ITO and tin oxide (SnOx) films are required to obtain the high experimental FFs of >80%. Optical and electrical losses in the tandem device are also addressed by quantum efficiencies (EQE, IQE) and reflectance simulation.

The power conversion efficiency (PCE) of perovskite/silicon tandem solar cells (PSTSCs) is expected to increase with optimized light management. In this work, we report on PSTSCs containing nanostructures enabling PCEs exceeding 26%. A hexagonal sinusoidal nanostructure with 750nm period was used. The structure was transferred into silicon by nanoimprint lithography and reactive ion etching. Perovskite top cells were deposited by spin-coating resulting in a full coverage of the nanostructure. PSTSC comprising these nanostructures yielded a steady-state PCE of 26.1% and a short-circuit current density of 19.5mA·cm−2.

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.

Through the optimization of the perovskite precursor composition and interfaces to selective contacts, we achieved a p i n type perovskite solar cell PSC with a 22.3 power conversion efficiency PCE . This is a new performance record for a PSC with an absorber bandgap of 1.63 eV. We demonstrate that the high device performance originates from a synergy between 1 an improved perovskite absorber quality when introducing formamidinium chloride FACl as an additive in the triple cation Cs0.05FA0.79MA0.16PbBr0.51I2.49 Cs MAFA perovskite precursor ink, 2 an increased open circuit voltage, VOC, due to reduced recombination losses when using a lithium fluoride LiF interfacial buffer layer, and 3 high quality hole selective contacts with a self assembled monolayer SAM of [2 9H carbazol 9 yl ethyl]phosphonic acid 2PACz on ITO electrodes. While all devices exhibit a high performance after fabrication, as determined from current density voltage, J V, measurements, substantial differences in device performance become apparent when considering longer term stability data. A reduced long term stability of devices with the introduction of a LiF interlayer is compensated for by using FACl as an additive in the metal halide perovskite thin film deposition. Optimized devices maintained about 80 of the initial average PCE during maximum power point MPP tracking for gt;700 h. We scaled the optimized device architecture to larger areas and achieved fully laser patterned series interconnected mini modules with a PCE of 19.4 for a 2.2 cm2 active area. A robust device architecture and reproducible deposition methods are fundamental for high performance and stable large area single junction and tandem modules based on PSCs

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

We present enhanced optical performance in perovskite/silicon tandem solar cells with smooth periodic nanotextures. Reflection losses in experimental devices are reduced by 1 mA/cm², enabling a power conversion efficiency >26%.

Summary Identification of electronic processes at buried interfaces of charge-selective contacts is crucial for photovoltaic and photocatalysis research. Here, transient surface photovoltage (SPV) is used to study the passivation of different hole-selective carbazole-based SAMs. It is shown that transient SPV and transient photoluminescence provide complementary information on charge transfer kinetics and trapping/de-trapping mechanisms, and that trap-assisted non-radiative recombination losses originate from electron trapping at the SAM-modified ITO/perovskite interface. The hole transfer rates and the density of interface electron traps, obtained by fitting SPV transients with a minimalistic kinetic model, depended strongly on the SAM's chemical structure, and densities of interface traps as low as 109 cm−2, on par with highly passivated c-Si surfaces, were reached for Me-4PACz, previously used in record perovskite/silicon tandem solar cells. The extracted hole transfer rate constants and interface trap densities correlated well with the corresponding fill factors and open-circuit voltages of high-efficiency solar cells.

Multi-junction solar cells provide an avenue to overcome fundamental efficiency limits of single-junction devices. The facile bandgap tunability of metal-halide perovskite solar cells renders them attractive building blocks for multi-junction architectures. Combinations with crystalline silicon and copper indium gallium selenide (CIGS) cells have been reported. All-perovskite tandem cells have likewise shown promising results. Meanwhile, narrow-gap non-fullerene acceptors (NFA) have revived the area of organic solar cells (OSCs) and unlocked skyrocketing efficiencies. Organic and perovskite semiconductors share similar processing technologies, which renders them attractive partners in multi junction architectures. As of yet, perovskite/organic tandem cells show subpar efficiencies of 20 per cent, limited by the low open circuit voltage (Voc) of wide-gap perovskite cells and losses introduced by the interconnect between the sub-cells. Here, we demonstrate two-terminal p-i-n perovskite/organic tandem cells with an efficiency of 23.5 per cent and a high Voc of 2.15 volts, operating near the levels predicted by a semi-empirical model. The perovskite sub-cells with optimized charge extraction layers afford an unsurpassed combination of a high Voc and fill-factor. The organic back-cells provide a high external quantum efficiency in the near-infrared. In surprising contrast to paradigmatic concerns about limited photostability of non-fullerene cells, we evidence an outstanding operational stability if excitons are predominantly generated on the NFA, which is the case in a tandem cell, where the illumination is spectrally filtered by the perovskite cell. A novel interconnect based on an ultra-thin (1.5 nanometers) metal like indium oxide layer offers unprecedented low optical/electrical losses. This work sets a new milestone for perovskite/organic tandem devices, that outperform the best p-i-n perovskite single junctions and are at par with perovskite/CIGS and all-perovskite multi-junctions. Perovskite/organic tandem architectures bear a realistic potential to reach an efficiency above 31%.

We show a monolithic perovskite/CIGS tandem solar cell with a certified PCE of 24.2% and a high V OC of 1.77 V, enabled by reduction of interface recombination. Using optical simulations, we further optimize the structure of the cell and compare it to perovskite/silicon tandem solar cells. The yearly energy yield of the perovskite/CIGS tandem is only 6% lower than that of the perovskite/silicon tandem, showing great potential of the perovskite/CIGS technology.

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.

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.

Funder: European Research Council; Id: http://dx.doi.org/10.13039/501100000781, Funder: Engineering and Physical Sciences Research Council; Id: http://dx.doi.org/10.13039/501100000266, Funder: European Union's Horizon 2020, Radiation‐resistant but cost‐efficient, flexible, and ultralight solar sheets with high specific power (W g−1) are the “holy grail” of the new space revolution, powering private space exploration, low‐cost missions, and future habitats on Moon and Mars. Herein, this study investigates an all‐perovskite tandem photovoltaic (PV) technology that uses an ultrathin active layer (1.56 µm) but offers high power conversion efficiency, and discusses its potential for high‐specific‐power applications. This study demonstrates that all‐perovskite tandems possess a high tolerance to the harsh radiation environment in space. The tests under 68 MeV proton irradiation show negligible degradation (22%. Using high spatial resolution photoluminescence (PL) microscopy, it is revealed that defect clusters in GaAs are responsible for the degradation of current space‐PV. By contrast, negligible reduction in PL of the individual perovskite subcells even after the highest dose studied is observed. Studying the intensity‐dependent PL of bare low‐gap and high‐gap perovskite absorbers, it is shown that the VOC, fill factor, and efficiency potentials remain identically high after irradiation. Radiation damage of all‐perovskite tandems thus has a fundamentally different origin to traditional space PV.

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 development of the simple synthesis schemes of organic semiconductors can have an important contribution to the advancement of related technologies. In particular, one of the fields where the high price of the hole amp; 8208;transporting materials may become an obstacle toward successful commercialization is perovskite solar cells. Herein, enamine amp; 8208;based materials that are capable of undergoing cross amp; 8208;linking due to the presence of two vinyl groups are synthesized. It is shown that new compounds can be thermally polymerized, making the films resistant to organic solvents. This can allow the use of a wet amp; 8208;coating process for the deposition of the perovskite absorber film, without the need for orthogonal solvents. Cross amp; 8208;linked films are used in perovskite solar cells, and, upon optimization of the film thickness, the highest power conversion efficiency of 18.1 is demonstrated

Solar cells based on metal halide perovskites have attracted tremendous attention due to the rapid increase in performance of single junctions and tandem solar cells. Recently, highest perovskite silicon tandem efficiencies are realized with front side polished silicon wafers or adapted microstructure of textured silicon solar cells. One way to integrate perovskite top cells on typical micrometer sized pyramidal structures, is conformal vacuum based perovskite deposition. Herein, fully vacuum based perovskite solar cells are developed on top of random pyramidal microtextured glass substrates with a pyramid size up to 9 mu m. This method allows improvement of the light management of the textured perovskite solar cell and resembles the typical pyramid topography of silicon solar cells as a step toward monolithic tandem integration. Moreover, to improve the quality of the perovskite on the textured substrates, three different methylammonium lead iodide MAPbI 3 films are tested by adjusting the rate ratio of the precursors. Optimized ratios for textured substrates with higher PbI2 rates enable a transient photoluminescence decay time above 0.75 mu s approaching that of planar substrates at around 1.2 mu s. Finally, a efficiency over 15 is achieved, which is, to the best of our knowledge, the first reported device on microscopically textured glass by co evaporated ion

The effect of sodium doping in NiO as a contact layer for perovskite solar cells is investigated. A combined X-ray diffraction and X-ray photoelectron spectroscopy analysis reveals that Na+ mostly segregates as NaOx/NaCl species around NiO crystallites, with the effect of reducing interface capacitance as revealed by impedance spectroscopy. Inspired by this finding, the NiO/perovskite interface in perovskite solar cells is modified via insertion of an ultrathin NaCl interlayer, which increases the NiO work-function by 0.3 eV. This leads to an increase of power conversion efficiency, approaching 18%, and open-circuit voltage due to a remarkable suppression of surface recombination, as revealed by photoluminescence analysis and light intensity–dependent electrical measurements.

The rapid rise of perovskite solar cells (PSCs) is increasingly limited by the available charge-selective contacts. This work introduces two new hole-selective contacts for p–i–n PSCs that outperform all typical p-contacts in versatility, scalability and PSC power-conversion efficiency (PCE). The molecules are based on carbazole bodies with phosphonic acid anchoring groups and can form self-assembled monolayers (SAMs) on various oxides. Besides minimal material consumption and parasitic absorption, the self-assembly process enables conformal coverage of arbitrarily formed oxide surfaces with simple process control. The SAMs are designed to create an energetically aligned interface to the perovskite absorber without non-radiative losses. For three different perovskite compositions, one of which is prepared by co-evaporation, we show dopant-, additive- and interlayer-free PSCs with stabilized PCEs of up to 21.1%. Further, the conformal coverage allows to realize a monolithic CIGSe/perovskite tandem solar cell with as-deposited, rough CIGSe surface and certified efficiency of 23.26% on an active area of 1 cm2. The simplicity and diverse substrate compatibility of the SAMs might help to further progress perovskite photovoltaics towards a low-cost, widely adopted solar technology.

Halide perovskites are emerging as revolutionary materials for optoelectronics. Their ionic nature and the presence of mobile ionic defects within the crystal structure have a dramatic influence on the operation of thin film devices such as solar cells, light emitting diodes, and transistors. Thin films are often polycrystalline and it is still under debate how grain boundaries affect the migration of ions and corresponding ionic defects. Laser excitation during photoluminescence PL microscopy experiments leads to formation and subsequent migration of ionic defects, which affects the dynamics of charge carrier recombination. From the microscopic observation of lateral PL distribution, the change in the distribution of ionic defects over time can be inferred. Resolving the PL dynamics in time and space of single crystals and thin films with different grain sizes thus, provides crucial information about the influence of grain boundaries on the ionic defect movement. In conjunction with experimental observations, atomistic simulations show that defects are trapped at the grain boundaries, thus inhibiting their diffusion. Hence, with this study, a comprehensive picture highlighting a fundamental property of the material is provided while also setting a theoretical framework in which the interaction between grain boundaries and ionic defect migration can be understood

Visionary quantum photonic networks need transform-limited single photons on demand. Resonance fluorescence on a quantum dot provides the access to a solid-state single photon source, where the environment is unfortunately the source of spin and charge noise that leads to fluctuations of the emission frequency and destroys the needed indistinguishability. We demonstrate a built-in stabilization approach for the photon stream, which relies solely on charge carrier dynamics of a two-dimensional hole gas inside a micropillar structure. The hole gas is fed by hole tunneling from field-ionized excitons and influences the energetic position of the excitonic transition by changing the local electric field at the position of the quantum dot. The standard deviation of the photon noise is suppressed by nearly 50 percent (noise power reduction of 6 dB) and it works in the developed micropillar structure for frequencies up to 1 kHz. This built-in feedback loop represents an easy way for photon noise suppression in large arrays of single photon emitters and promises to reach higher bandwidth by device optimization., Comment: 17 pages, 4 figures

The structural phases and optoelectronic properties of coevaporated CsPbI 3 thin films with a wide range of [CsI]/[PbI 2 ] compositional ratios are investigated using high throughput experimentation and gradient samples. It is found that for CsI-rich growth conditions, CsPbI 3 can be synthesized directly at low temperature into the distorted perovskite γ-CsPbI 3 phase without detectable secondary phases. In contrast, PbI 2 -rich growth conditions are found to lead to the non-perovskite δ-phase. Photoluminescence spectroscopy and optical-pump THz-probe mapping show carrier lifetimes larger than 75 ns and charge carrier (sum) mobilities larger than 60 cm 2 V −1 s −1 for the γ-phase, indicating their suitability for high efficiency solar cells. The dependence of the carrier mobilities and luminescence peak energy on the Cs-content in the films indicates the presence of Schottky defect pairs, which may cause the stabilization of the γ-phase. Building on these results, p–i–n type solar cells with a maximum efficiency exceeding 12% and high shelf stability of more than 1200 h are demonstrated, which in the future could still be significantly improved, judging on their bulk optoelectronic properties.