In this work, the authors realize stable and highly efficient wide‐bandgap perovskite solar cells that promise high power conversion efficiencies (PCE) and are likely to play a key role in next generation multi‐junction photovoltaics (PV). This work reports on wide‐bandgap (≈1.72 eV) perovskite solar cells exhibiting stable PCEs of up to 19.4% and a remarkably high open‐circuit voltage (VOC) of 1.31 V. The VOC‐to‐bandgap ratio is the highest reported for wide‐bandgap organic−inorganic hybrid perovskite solar cells and the VOC also exceeds 90% of the theoretical maximum, defined by the Shockley–Queisser limit. This advance is based on creating a hybrid 2D/3D perovskite heterostructure. By spin coating n‐butylammonium bromide on the double‐cation perovskite absorber layer, a thin 2D Ruddlesden–Popper perovskite layer of intermediate phases is formed, which mitigates nonradiative recombination in the perovskite absorber layer. As a result, VOC is enhanced by 80 mV.

application-oriented research like process engineering and upscaling is observed. [1][2][3][4][5] Even though other optoelectronic devices like light emitting diodes and lasers are being researched, [6][7][8][9][10][11][12][13] perovskite-based photovoltaics (PV) is the key technology driving the fast emergence of perovskitebased optoelectronics. Recently, power conversion efficiencies (PCEs) close to 24% were demonstrated for perovskite PV, exceeding the PCEs of established thinfilm technologies. [14] Despite the rapid progress in terms of PCE, one key challenge of perovskite-based PV is still its low stability under realistic outdoor stress conditions-temperature, humidity, and ultraviolet (UV) radiation. A significant advance toward more stable devices was demonstrated by engineering the composition of the large cation site of the perovskite crystal structure and by including low-dimensional perovskite interlayers and passivation layers. [15][16][17][18][19][20] Further advances in stability are based on the charge extracting materials and their interfaces with the perovskite absorber layers. [21][22][23] Most reported record PCEs are still based on highly expensive organic hole transport layer (HTL) materials like 2,2′,7,7′-tetrakis[N,N-di (4methoxyphenyl)amino]-9,9′-spirobifluorene (spiro-MeOTAD) or poly[bis(4-phenyl)(2,4,6-trimethylphenyl)amine] (PTAA). [20,24,25] Although these materials result in good performance on short High-quality charge carrier transport materials are of key importance for stable and efficient perovskite-based photovoltaics. This work reports on electron-beam-evaporated nickel oxide (NiO x ) layers, resulting in stable power conversion efficiencies (PCEs) of up to 18.5% when integrated into solar cells employing inkjet-printed perovskite absorbers. By adding oxygen as a process gas and optimizing the layer thickness, transparent and efficient NiOx hole transport layers (HTLs) are fabricated, exhibiting an average absorptance of only 1%. The versatility of the material is demonstrated for different absorber compositions and deposition techniques. As another highlight of this work, all-evaporated perovskite solar cells employing an inorganic NiO x HTL are presented, achieving stable PCEs of up to 15.4%. Along with good PCEs, devices with electron-beam-evaporated NiO x show improved stability under realistic operating conditions with negligible degradation after 40 h of maximum power point tracking at 75 °C. Additionally, a strong improvement in device stability under ultraviolet radiation is found if compared to conventional perovskite solar cell architectures employing other metal oxide charge transport layers (e.g., titanium dioxide). Finally, an all-evaporated perovskite solar mini-module with a NiO x HTL is presented, reaching a PCE of 12.4% on an active device area of 2.3 cm 2 .

Monolithic all-perovskite tandem photovoltaics promise to combine low-cost and high-efficiency solar energy harvesting with the advantages of all-thin-film technologies. To date, laboratory-scale all-perovskite tandem solar cells have only been fabricated using non-scalable fabrication techniques. In response, this work reports on laser-scribed all-perovskite tandem modules processed exclusively with scalable fabrication methods (blade coating and vacuum deposition), demonstrating power conversion efficiencies up to 19.1% (aperture area, 12.25 cm2; geometric fill factor, 94.7%) and stable power output. Compared to the performance of our spin-coated reference tandem solar cells (efficiency, 23.5%; area, 0.1 cm2), our prototypes demonstrate substantial advances in the technological readiness of all-perovskite tandem photovoltaics. By means of electroluminescence imaging and laser-beam-induced current mapping, we demonstrate the homogeneous current collection in both subcells over the entire module area, which explains low losses (<5%rel) in open-circuit voltage and fill factor for our scalable modules.

This paper reports on the impact of outdoor temperature variations on the performance of organo metal halide perovskite solar cells (PSCs). It shows that the open-circuit voltage ( V) of a PSC decreases linearly with increasing temperature. Interestingly, in contrast to these expected trends, the current density ( J) of PSCs is found to decline strongly below 20% of the initial value upon cycling the temperatures from 10 to 60 °C and back. This decline in the current density is driven by an increasing series resistance and is caused by the fast temperature variations as it is not apparent for solar cells exposed to constant temperatures of the same range. The effect is fully reversible when the devices are kept illuminated at an open circuit for several hours. Given these observations, an explanation that ascribes the temperature variation-induced performance decline to ion accumulation at the contacts of the solar cell because of temperature variation-induced changes of the built-in field of the PSC is proposed. The effect might be a major obstacle for perovskite photovoltaics because the devices exposed to real outdoor temperature profiles over 4 h showed a performance decline of >15% when operated at a maximum power point.

Perovskite solar cells (PSCs) demonstrate excellent power conversion efficiencies (PCEs) but face severe stability challenges. One key degradation mechanism is exposure to ultraviolet (UV) light. However, the impact of different UV bands is not yet well established. Here, we systematically study the stability of PSCs on the basis of a methylammonium lead iodide (CHNHPbI) absorber exposed to (i) 310-317 (UV-B range) and (ii) 360-380 nm (UV-A range), under accelerated conditions. We demonstrate that the investigated UV-B band is detrimental to the stability of PSCs, resulting in PCE degradation by more than 50% after an exposure period >1700 sun-hours. This finding is valid for architectures with a range of electron transport layers, including SnO, compact-TiO, electron-beam TiO, and nanoparticle-TiO. We also show that photodegradation is apparent for high, as well as for low illumination intensities of UV-B light, but not for illumination with UV-A wavelengths. Finally, we show that degradation of PSCs is preventable at the cost of a small fraction of photocurrent by using UV-filtering or luminescent downshifting layers.

Interfacial engineering is the key to high‐performance perovskite solar cells (PSCs). While a wide range of fullerene interlayers are investigated for Pb‐based counterparts with a bandgap of >1.5 eV, the role of fullerene interlayers is barely investigated in Sn‐Pb mixed narrow‐bandgap (NBG) PSCs. In this work, two novel solution‐processed fullerene derivatives are investigated, namely indene‐C60‐propionic acid butyl ester and indene‐C60‐propionic acid hexyl ester (IPH), as the interlayers in NBG PSCs. It is found that the devices with IPH‐interlayer show the highest performance with a remarkable short‐circuit current density of 30.7 mA cm−2 and a low deficit in open‐circuit voltage. The reduction in voltage deficit down to 0.43 V is attributed to reduced non‐radiative recombination that the authors attribute to two aspects: 1) a higher conduction band offset of ≈0.2 eV (>0 eV) that hampers charge‐carrier‐back‐transfer recombination; 2) a decrease in trap density at the perovskite/interlayer/C60 interfaces that results in reduced trap‐assisted recombination. In addition, incorporating the IPH interlayer enhances charge extraction within the devices that results in considerable enhancement in short‐circuit current density. Using a NBG device with an IPH interlayer, a respectable power conversion efficiency of 24.8% is demonstrated in a four‐terminal all‐perovskite tandem solar cell.

This work studies spontaneous enhancement in power conversion efficiency of multi-cation-halide perovskite solar cells which occurs days after device fabrication.

enormous interest in perovskite-based multi-junction photovoltaics (PV). [1] To go beyond Shockley-Queisser radiative efficiency limit for single-junction solar cells, wide-bandgap (WBG) perovskite top solar cells (E G > 1.6 eV) [5] are combined with high-efficiency low-bandgap (LBG) bottom solar cells made from Si, [6] CIGS [7] or LBG (E G < 1.3 eV) perovskite devices. [8][9][10] While tandem PV technologies based on market-dominant crystalline Si and CIGS bottom solar cells have recently demonstrated PCEs exceeding 28%, [6,11] all-perovskite tandem solar cells are still less advanced. In comparison to single junction PSCs, all-perovskite tandem solar cells still lack behind with record PCEs of 23.1% [12] and 25% [12] for of all-perovskite two-terminal (2T) and four-terminal (4T) tandem solar cells, respectively.The key challenges hindering the progress of all-perovskite tandem solar cells are the low performance and stability of the LBG perovskite bottom solar cells. To resolve these challenges, previous studies on LBG perovskite thin films addressed compositional engineering of the perovskite, strategies to improve the thin-film morphology, and routes to enhance the optical and electrical properties. [8,10,[12][13][14][15] LBG All-perovskite multijunction photovoltaics, combining a wide-bandgap (WBG) perovskite top solar cell (E G ≈1.6-1.8 eV) with a low-bandgap (LBG) perovskite bottom solar cell (E G < 1.3 eV), promise power conversion efficiencies (PCEs) >33%. While the research on WBG perovskite solar cells has advanced rapidly over the past decade, LBG perovskite solar cells lack PCE as well as stability. In this work, vacuum-assisted growth control (VAGC) of solution-processed LBG perovskite thin films based on mixed Sn-Pb perovskite compositions is reported. The reported perovskite thin films processed by VAGC exhibit large columnar crystals. Compared to the well-established processing of LBG perovskites via antisolvent deposition, the VAGC approach results in a significantly enhanced charge-carrier lifetime. The improved optoelectronic characteristics enable high-performance LBG perovskite solar cells (1.27 eV) with PCEs up to 18.2% as well as very efficient four-terminal all-perovskite tandem solar cells with PCEs up to 23%. Moreover, VAGC leads to promising reproducibility and potential in the fabrication of larger active-area solar cells up to 1 cm 2 .In recent years, hybrid organic-inorganic perovskite materials attracted tremendous attention due to their outstanding optoelectronic and piezoelectric properties. [1][2][3] The optoelectronic properties of the perovskite materials enables power conversion efficiencies (PCEs) as high as 25.2% in singlejunction perovskite thin-film solar cells. [4] Moreover, the wide range of bandgaps (E G ) of this class of materials generates Adv. Energy perovskite thin films are realized by careful compositional engineering, incorporating Sn at the site of Pb in multication perovskite crystal structures. [8,10,13] In this regard, the exact ratio of Sn to Pb is criti...