Tandem solar cells are the next step in the photovoltaic (PV) evolution due to their higher power conversion efficiency (PCE) potential than currently dominating, but inherently limited, ...single‐junction solar cells. With the emergence of metal halide perovskite absorber materials, the fabrication of highly efficient tandem solar cells, at a reasonable cost, can significantly impact the future PV landscape. The perovskite‐based tandem solar cells have already shown that they can convert light more efficiently than their standalone sub‐cells. However, to reach PCEs over 30%, several challenges have to be overcome and the understanding of this fascinating technology has to be broadened. In this review, the main scientific and engineering challenges in the field are presented, alongside a discussion of the current status of three main perovskite tandem technologies: perovskite/silicon, perovskite/CIGS, and perovskite/perovskite tandem solar cells. A summary of the advanced structural, electrical, optical, radiative, and electronic characterization methods as well as simulations being utilized for perovskite‐based tandem solar cells is presented. The main findings are summarized and the strength of the techniques to overcome the challenges and gain deeper knowledge for further performance improvement is assessed. Finally, the PCE potential in different experimental and theoretical limits is compared with an aim to shed light on the path towards overcoming the 30% efficiency threshold for all of the three herein reviewed tandem technologies.
In this comprehensive review, the main challenges and the current status of perovskite/silicon, perovskite/CIGS, and perovskite/perovskite tandem technologies are presented. A specific focus is set on advanced characterization methods as well as simulations being utilized for perovskite‐based tandem solar cells to overcome the challenges and gain deeper knowledge to further improve device performance. Finally, the efficiency potentials in different experimental and theoretical limits are compared and pathways toward 35% efficiency are outlined.
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 (PbI2). This substrate temperature-dependent evaporation behavior of MAI is also transferred to the co-evaporation process and can directly influence the perovskite composition. We demonstrate that the optimal substrate temperature window for perovskite deposition is close to room temperature. At high temperature, not enough MAI for precise stoichiometry is incorporated even with very high MAI rates. While, at temperatures below −25 °C, the conversion of MAI with PbI2 is inhibited, and an amorphous yet unreacted film is formed. We observe that perovskite composition and morphology vary widely between the organic hole-transport layers (HTLs) PTAA and MeO-2PACz. For all substrate temperatures, MeO-2PACz enables higher solar cell PCEs than PTAA. Through the combination of vapor-deposited perovskites and a self-assembled monolayer, we achieve a stabilized power conversion efficiency of 20.6%, which is the first reported PCE above 20% for evaporated perovskite solar cells in p-i-n architecture.
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 −0.38% K–1 notably higher than the one from the perovskite subcell (−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.
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 molecule 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 textured 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.
A novel concept for the formation of the hole selective layer in efficient perovskite solar cells is presented. Carbazole‐based material is synthesized and used for the formation of a self‐assembled monolayer on top of the indium tin oxide transparent conductive substrate. Power conversion efficiency as high as 17.8% is achieved.
Tandem solar cells that pair silicon with a metal halide perovskite are a promising option for surpassing the single-cell efficiency limit. We report a monolithic perovskite/silicon tandem with a ...certified power conversion efficiency of 29.15%. The perovskite absorber, with a bandgap of 1.68 electron volts, remained phase-stable under illumination through a combination of fast hole extraction and minimized nonradiative recombination at the hole-selective interface. These features were made possible by a self-assembled, methyl-substituted carbazole monolayer as the hole-selective layer in the perovskite cell. The accelerated hole extraction was linked to a low ideality factor of 1.26 and single-junction fill factors of up to 84%, while enabling a tandem open-circuit voltage of as high as 1.92 volts. In air, without encapsulation, a tandem retained 95% of its initial efficiency after 300 hours of operation.
Highly efficient perovskite based solar cells have the potential to be a game-changing solar array technology for space applications that can be flexible, truly roll-able, ultra-lightweight and ...highly stowable. Outside earth's magnetic field, however, ionizing radiation causes localized defect states that accumulate and ultimately cause the failure of electronic devices. This study, assesses the radiation hardness of the widely used triple cation based perovskite absorber material, namely Cs
0.05
MA
0.17
FA
0.83
Pb(I
0.83
Br
0.17
)
3
employing 20 and 68 MeV proton irradiation. Therefore,
in situ
measurements of the degradation of the proton induced current as well as the photovoltaic performance during proton irradiation are used as two independent metrics. Both measurements suggest that triple cation perovskites even exceed the radiation hardness of SiC, which is a material often proposed to possess an excellent radiation hardness. Our optimized Cs
0.05
MA
0.17
FA
0.83
Pb(I
0.83
Br
0.17
)
3
based space solar cells reach efficiencies of 18.8% under AM0 illumination and maintain 95% of their initial efficiency even after irradiation with protons at an energy 68 MeV and a total dose of 10
12
p per cm
2
. Degradation under 20 MeV proton irradiation is even lower. Despite the negligible impact on solar cell device performance, this study identifies that proton irradiation is changing the recombination kinetics under low excitation densities profoundly. Dark capacitance-voltage and current-voltage characteristics, photoluminescence spectra as well as photoluminescence and
V
oc
decays are analyzed in depth. Surprisingly, two fold prolonged PL and
V
oc
decay times are observed after proton irradiation. Often, such prolongations are attributed to a reduced charge recombination. Our kinetic model, precisely describing the observed time evolution after photoexcitation, however, establishes the prolonged release of trapped minority charge carriers from proton-radiation induced trap states.
Although highly energetic proton irradiation forms localized trap states in triple cation perovskites, solar cells possess exceptional radiation hardness.
Perovskite solar cells (PSC) have shown that under laboratory conditions they can compete with established photovoltaic technologies. However, controlled laboratory measurements usually performed do ...not fully resemble operational conditions and field testing outdoors, with day‐night cycles, changing irradiance and temperature. In this contribution, the performance of PSCs in the rooftop field test, exposed to real weather conditions is evaluated. The 1 cm2 single‐junction devices, with an initial average power conversion efficiency of 18.5% are tracked outdoors in maximum power point over several weeks. In parallel, irradiance and air temperature are recorded, allowing us to correlate outside factors with generated power. To get more insight into outdoor device performance, a comprehensive set of laboratory measurements under different light intensities (10% to 120% of AM1.5) and temperatures is performed. From these results, a low power temperature coefficient of −0.17% K−1 is extracted in the temperature range between 25 and 85 °C. By incorporating these temperature‐ and light‐dependent PV parameters into the energy yield model, it is possible to correctly predict the generated energy of the devices, thus validating the energy yield model. In addition, degradation of the tested devices can be tracked precisely from the difference between measured and modelled power.
In this paper, laboratory and rooftop performance of perovskite solar cells under changing temperature and irradiance is analyzed. By integrating laboratory data trends and measured weather data into optical energy yield model, the temperature‐dependent energy yield model is developed and validated, and can be used to predict generated energy of perovskite solar cells or track their degradation during field testing.
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 cm
2
. The simplicity and diverse substrate compatibility of the SAMs might help to further progress perovskite photovoltaics towards a low-cost, widely adopted solar technology.
We introduce new hole-selective contacts for next-generation perovskite photovoltaics and point to design paths for molecular engineering of perfect interfaces.
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.
We present a highly efficient monolithic perovskite/silicon tandem solar cell and analyze the tandem performance as a function of photocurrent mismatch with important implications for future device and energy yield optimizations.
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