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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...

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

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.

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

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 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.

We have measured the spin relaxation time of an excited two-electron spin-triplet state into its singlet ground state in self-assembled InAs/GaAs quantum dots. We use a time-resolved measurement scheme that combines transconductance spectroscopy with spin-to-charge conversion to address the |s↑,p↑〉 triplet state, where one electron is in the quantum dot s-shell and a second one in the p-shell. The evaluation of the state-selective tunneling times from the dots into a nearby two-dimensional electron gas allows us to determine the s- and p-shell occupation and extract the relaxation time from a rate equation model. A comparably long triplet-to-singlet spin relaxation time of 25 μs is found.

The unprecedented emergence of perovskite based solar cells PSCs has been accompanied by an intensive search of suitable materials for charge selective contacts. For the first time a hole transporting self assembled monolayer SAM as the dopant free hole selective contact in p i n PSCs is used and a power conversion efficiency of up to 17.8 with average fill factor close to 80 and undetectable parasitic absorption is demonstrated. SAM formation is achieved by simply immersing the substrate into a solution of a novel mole cule V1036 that binds to the indium tin oxide surface due to its phosphonic anchoring group. The SAM and its modifications are further characterized by Fourier transform infrared and vibrational sum frequency generation spectroscopy. In addition, photoelectron spectroscopy in air is used for measuring the ionization potential of the studied SAMs. This novel approach is also suitable for achieving a conformal coverage of large area and or tex tured substrates with minimal material consumption and can potentially be extended to serve as a model system for substrate based perovskite nucleation and passivation control. Further gains in efficiency can be expected upon SAM optimization by means of molecular and compositional engineering

We present a new strategy for highly efficient perovskite/CIGSe monolithic tandem solar cells, fabricated directly on top of a rough CIGSe surface. This was enabled by conformally depositing the metal oxide NiOx by atomic layer deposition, as confirmed by TEM/EDX measurements. The resulting limiting NiOx/perovskite interface was improved by spin-coating additional thin layer of p-type polymer PTAA, thus forming a NiOx/PTAA hole selective bilayer. The fabricated tandem device has a 21.6% power conversion efficiency on 0.778 cm2, stable over 10 minutes of maximum power point tracking. The device performance is further analyzed by absolute photoluminescence measurements from which a VOC contribution of each subcell to the tandem VOC can be estimated.