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

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

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

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

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

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

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

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

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

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

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

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

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

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

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

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

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

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

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

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

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

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

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

The superstrate configuration of Cu(In,Ga)Se2 (CIGS) photovoltaic devices exhibits the potential for improved light harvesting compared to the standard substrate configuration. Due to the limited power conversion efficiency of superstrate devices caused by the poor hetero-interface between the p-type CIGS and the n-type component, these advantages have not been fully considered so far. This work shows that the superstrate configuration can significantly improve the light management within CIGS devices. Experimentally, it is shown that the electric and optical properties of ZnO window layer strongly improve during the CIGS deposition, allowing the use of structured ZnO layers for efficient light-trapping. A highly reflective and scattering back contact is realized by using the high work function material MoO3−x for the hole-transport layer in combination with a low work function Ag metal layer. Combined with the unique Ga gradient achievable in the superstrate configuration, simulation results show that a strong reduction of the CIGS layer thickness is possible while increasing the power conversion efficiency. This proof of concept highlights the appeal of the superstrate configuration for the future of cost-effective CIGS solar cell production.

This work reports a laser firing technique applied to completed silicon heterojunction interdigitated back contact solar cells in order to lower contact resistance. Previously, the implementation of a-Si:H(i) at the electron contact of polycrystalline silicon solar cells on glass substrates led to an increase in series resistance. The cell architecture with the current record efficiency of 14.2% (with illumination through glass) utilizes only an a-Si:H(n+) layer and 2–2.9 mA cm−2 of short circuit current density is lost due to electrical shading under the electron contact [1,2]. The goal of implementing an a-Si:H(i) layer and laser firing at this contact is to achieve low contact resistance at fired spots while preserving a-Si:H(i) passivation in unfired regions. After the laser firing, VOC was retained, while up to 14% absolute increase in FF was obtained with a mere 0.2 mA cm−2 loss in JSC. In the best performing cell, a 72.1% FF was achieved with a 0.7 mA cm−2 loss in JSC. Two laser sources were used to first ablate a part of the silver contact metal, and then to laser fire through the Si(n)/a-Si:H(i/n+)/ITO/Ag contact. The optimal laser fluence was found to be 1.1–0.5 J cm−2 (355 nm, picosecond pulse duration) and 4.4–5.2 J cm−2 (532 nm, nanosecond pulse duration), respectively. The upper limit on specific contact resistance in the laser fired spots was calculated to be 38 ± 20 mΩ cm 2 as a conservative estimate.

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.

P2 laser patterning of the perovskite layer for serial monolithic integration was systematically investigated by laser ablation using nanosecond laser pulses at varied laser fluences. The correlation of the laser impact to the morphology, composition and electrical functionality was analyzed in detail by several surface-analytical techniques. It is found that material removal via stress-assisted ablation is strongly influenced by thermal processes. The formation of PbI 2 containing residuals was evidenced, presumably causing contact resistance losses through the P2 interconnect. From these results loss factors in laser-based serial interconnection of perovskite solar cells were identified, allowing for process optimization for upscaling to industrial module sizes.

The liquid phase crystallization (LPC) of silicon is an emerging technology for fabricating 10 − 20 µm thin multi-crystalline silicon layers on glass. LPC silicon solar cells exhibit similar electronic performance to multi-crystalline wafer-based devices. Due to the reduced absorber thickness, however, effective measures for light trapping have to be taken. We present tailor-made micro-structures for light trapping at the LPC silicon back-side, whereby a nano-imprinted resist layer serves as a three-dimensional etching mask in subsequent reactive ion etching. Contrary to state-of-the-art random pyramid textures produced by wet-chemical etching, this method allows to produce tailor-made textures independent of grain orientation. Differently shaped micro-textures were replicated in LPC silicon. Absorptance and external quantum efficiency of periodic honeycomb patterns and random pyramids were found to be equivalent. Thus, the method enables the potential to further optimize light trapping in LPC silicon solar cells.

Tandem solar cells combining silicon and perovskite absorbers have the potential to outperform state-of-the-art high efficiency silicon single junction devices. However, the practical fabrication of monolithic silicon/perovskite tandem solar cells is challenging as material properties and processing requirements such as temperature restrict the device design. Here, we fabricate an 18% efficient monolithic tandem cell formed by a silicon heterojunction bottom-and a perovskite top-cell enabling a very high open circuit voltage of 1.78 V. The monolithic integration was realized via low temperature processing of the semitransparent perovskite sub-cell where an energetically aligned electron selective contact was fabricated by atomic layer deposition of tin oxide. The hole selective, transparent top contact was formed by a stack of the organic hole transport material spiro-OMeTAD, molybdenum oxide and sputtered indium tin oxide. The tandem cell design is currently limited by the photo-current generated in the silicon bottom cell that is reduced due to reflectance losses. Based on optical modelling and first experiments, we show that these losses can be significantly reduced by combining optical optimization of the device architecture including light trapping approaches.

We present a detailed analysis of the photo-current potentials and losses in thin film crystalline silicon solar cells on glass. The effects of texturing the silicon backside, applying a diffuse back reflector and a textured anti-reflection foil were analysed. Light beam induced current measurements were used to determine the losses due to local effects like the absorber contact, cracks in the absorber and grain boundaries. Detailed loss analysis in combination with ray-tracing simulations showed that the maximum light trapping potential imposed by geometrical optics has nearly been achieved. The photocurrent losses due to incomplete carrier collection and parasitic absorption were accounted for using a theoretical model. For the investigated, textured, n-doped cell with reflector and anti-reflection foil, the short circuit current density ( J SC ) was 28.9 mA/cm 2 and the main loss factors were direct reflection (3.4 mA/cm 2 ), electrical shading effects due to the absorber contact (3.1 mA/cm 2 ) and incomplete carrier collection due to surface/bulk recombination (1.6 mA/cm 2 ). Using the presented light trapping scheme we obtained the following efficiencies: 11.8% for a p-doped and 12.1% for an n-doped crystalline silicon absorber. Finally, the potentials for efficiencies beyond 14% are discussed.

Recent progress in Liquid Phase Crystallization (LPC) of silicon enabled reaching a material quality of thin-film silicon solar cells on glass comparable to multicrystalline silicon wafers. However, decreasing the absorber thickness requires taking measures for efficient coupling and trapping light into the solar cell device. Here, we successfully integrated different periodic sub-micrometer sized structures at the sun-facing air-glass superstrate interface of 5 x 5 cm 2 LPC silicon thin-film solar cells by nanoimprint lithography. These structured superstrates were modularly attached to the device and found to provide both, anti-reflective and scattering properties. In this study, the influence of the structure type and geometry is examined. With the structures used an enhancement in short-circuit current density of + 5% (relative) compared to the planar device could be achieved.

Thin crystalline silicon solar cells prepared directly on glass substrates by means of liquid-phase crystallization of the absorber utilize only a small fraction of the silicon material used by standard wafer-based silicon solar cells. The material consists of large crystal grains of up to square centimeter area and results in solar cells with open-circuit voltages of 650 mV, which is comparable with results achieved with multi-crystalline silicon wafers. We give a brief status update and present new results on the electronic interface and bulk properties. The interrelation between surface passivation and additional hydrogen plasma passivation is investigated for p-type and n-type absorbers with different doping concentrations. Internal quantum efficiency measurements from both sides on bifacial solar cells are used to extract the bulk-diffusion length and surface-recombination velocity. Finally, we compare various types of solar cell devices based on 10 µm thin crystalline silicon, where conversion efficiencies of 11–12% were achieved with p–type and n-type liquid-phase crystallized absorbers on glass. Copyright © 2015 John Wiley & Sons, Ltd.

We recently demonstrated how the short-circuit current density of an a-Si:H/c-Si heterojunction solar cell can be significantly improved to above 40 mA/cm2 by replacing the standard a-Si:H(p) emitter by a silicon oxide emitter containing p-doped silicon nanocrystallites. While we could obtain a conversion efficiency of 20.3%, the cell suffered from a lower fill factor of 72.9%, compared with 77.0% for our standard process. In this paper, we address this issue both theoretically and experimentally. We found that a thin (∼3 nm) highly doped nanocrystalline silicon layer on top of the emitter can greatly improve the fill factor. Using 1-D device simulation, we explain the prevalent loss mechanism, which originates mostly from poor tunnel recombination at the transparent conducting oxide/emitter interface rather than in the bulk of the emitter. We suspect that have their origin in the lower effective dopant concentration of the nanocrystalline silicon oxide emitter. From the model, implications for further developments can be derived.

The crystallization process of hydrogen doped In2O3:H (IOH) films is investigated with energy-dispersive X-ray diffraction measurements. At annealing temperatures between 125 and 150 °C crystallization of 220 nm thin films occurs within only 2 min, and the percentage of the crystalline phase does not change anymore when the temperature is raised above the crystallization temperature of 150 °C. Maximum electron mobilities above 100 cm2/Vs have been reached after crystallization. The IOH films were integrated as front contact into amorphous/crystalline silicon heterojunction cells and compared to In2O3:Sn (ITO) front contacts. Cells with ITO/IOH bilayer front contacts show a slightly lower open circuit voltage because of the a-Si:H passivation layer degradation caused by the longer annealing process needed for the crystallization of the bilayers, while all cells reach total area efficiencies around 20%. IOH films were also implemented as silver free back contact for μc-Si:H cells, and show higher short-circuit current densities than ZnO:Al back contacts because of the higher near-infra-red transmission of IOH.

Liquid-phase crystallization (LPC) has proven to be a suitable method to grow large-grained silicon films on commercially well-available glass substrates. Zone-melting crystallization with high-energy-density line sources such as lasers or electron beams enabled polycrystalline grain growth with wafer equivalent morphology. However, the electronic quality is strongly affected by the material used as the interlayer between the glass and the silicon absorber. Open-circuit voltages above 630 mV, and efficiencies up to 11.8% were demonstrated using n-type absorbers on a sputtered interlayer comprising a triple stack of SiO2/SiN $_{x}$ /SiO2. In this study, we present our results to further improve the device performance by investigating the influence of the interlayer on the open-circuit voltage of the devices and characterize the properties of the absorber and interface using bias light-dependent quantum efficiency data and transmission electron microscopy (TEM) images. Finally, we investigate the applicability of aluminum oxide (Al2 O3) for passivation of p-type LPC absorbers.

Liquid phase crystallization of silicon is a promising technology to grow crystalline silicon thin films on glass. It has already been demonstrated that open circuit voltages of up to 656 mV and efficiencies of up to 11.8% can be achieved by this technique. Nevertheless further improvements are required to become competitive with wafer based silicon solar cells. A possibility to improve the quality is to enlarge the grain size and to control the crystallographic orientation of the resulting layers. While a preferential {100} surface orientation can be triggered utilizing suitable crystallization parameters, the in-plane orientation still remains random. Also the grain size stays within the same range. By introducing a local monocrystalline seed at the beginning of the crystallization process, we are able to control both the surface and the in-plane orientation of the silicon films. In addition the grain size is significantly increased in scanning direction and only limited by the substrate size of 5 cm. This high morphological quality is accompanied by an improved electrical quality confirmed by photoluminescence imaging and Hall measurements. This is a big step towards the final goal to directly grow monocrystalline silicon thin films on glass substrates.

In this study we developed a hydrogenated nanocrystalline silicon oxide (p)nc-SiO x :H as an emitter window layer for silicon heterojunction solar cells. We investigated the variation of refractive index and crystalline volume fraction at different growth conditions by Plasma Enhanced Chemical Vapor Deposition (PECVD) and we show that combining a low refractive index (n ∼ 2.65) and low parasitic absorption the (p)nc-SiO x :H emitter can replace the standard (p)a-Si:H, which leads to a short circuit current increase of up to 4%. We also show a method to reduce the incubation layer thickness in the initial stage of growth using a CO 2 plasma treatment of the intrinsic amorphous layer surface prior to the emitter deposition. Lifetime measurements prove that the plasma treatment and the emitter layer deposition did not compromise the passivation layer quality. Moreover, in order to improve the p-emitter/n-type TCO contact, a highly doped nc-Si:H layer is implemented on top of the emitter, which leads to lower series resistance (R s,light ) and higher fill factor (FF) without affecting the open circuit voltage (V oc ).

We fabricated interdigitated back-contact silicon hetero-junction solar cells based on thin-film absorbers on glass. The Si absorbers were directly deposited on the glass and crystallized using liquid phase crystallization. To compare whether our contact system is applicable to a wide range of initial absorber conditions two different types of precursors were prepared with absorber thicknesses between 2.5-9 μm. Furthermore, glass superstrates, doping densities and interlayer stacks were varied. With a KOH random pyramid light trapping texture at the back more than 30 mA/cm 2 were achieved on an electron beam evaporated precursor material and 655 mV on a PECVD precursor material.

We investigate the influence of the barrier type and the absorber doping on the open-circuit voltage of liquid phase-crystallized silicon solar cells on glass. It was found that the use of n-type instead of p-type substrates is the major reason for the recently reported boost of the open-circuit voltage ( $V_{\rm OC}$ ) up to values of 656 mV, which is by far exceeding the previously reported $V_{\rm OC}$ values of crystalline silicon solar cells on glass. Despite the high doping, locally, an internal quantum efficiency of $\text{90\%}$ can be achieved. Therewith, efficiencies of $\text{16\%}$ and up should be possible.

Emerging liquid phase crystallization (LPC) techniques recently rendered a possible substantial progress in the fabrication of high quality crystalline silicon thin-film solar cells on glass. The implementation of an efficient light trapping texture into such LPC silicon devices is still challenging as an excellent bulk material quality and well-passivated interfaces have to be guaranteed. In this paper we present recent advances in light management for LPC silicon thin-film solar cells on imprinted glasses. A double-sided 2 µm periodic texture is realized by sandwiching the silicon film during the electron-beam induced crystallization process between an imprinted glass substrate coated with silicon oxide and a silicon oxide capping layer. Amorphous-crystalline silicon (a-Si:H/c-Si) heterojunction solar cells with single sided contacting scheme are fabricated. Textured prototype devices and simultaneously processed planar solar cells exhibit a comparable electronic material quality featuring open circuit voltages above 550 mV and efficiencies up to 8.1%. Optical absorption properties of 10 µm thick double-side textured silicon films even predict maximum achievable short circuit current densities in solar cells up to 38 mA/cm2 assuming zero parasitic absorption.

We present grazing incidence X-ray fluorescence (GIXRF) experiments on 3D periodically textured interfaces of liquid phase crystallized silicon thin-film solar cells on glass. The influence of functional layers (SiOx or SiOx/SiCx) – placed between glass substrate and silicon during crystallization – on the final carbon and oxygen contaminations inside the silicon was analyzed. Baring of the buried structured silicon surface prior to GIXRF measurement was achieved by removal of the original nano-imprinted glass substrate by wet-chemical etching. A broad angle of incidence distribution was determined for the X-ray radiation impinging on this textured surface. Optical simulations were performed in order to estimate the incident radiation intensity on the structured surface profile considering total reflection and attenuation effects. The results indicate a much lower contamination level for SiOx compared to the SiOx/SiCx interlayers, and about 25% increased contamination when comparing structured with planar silicon layers, both correlating with the corresponding solar cell performances.

Singlet exciton fission is an exciton multiplication process that occurs in certain organic materials, converting the energy of single highly-energetic photons into pairs of triplet excitons. This could be used to boost the conversion efficiency of crystalline silicon solar cells by creating photocurrent from energy that is usually lost to thermalisation. An appealing method of implementing singlet fission with crystalline silicon is to incorporate singlet fission media directly into a crystalline silicon device. To this end, we developed a solar cell that pairs the electron-selective contact of a high-efficiency silicon heterojunction cell with an organic singlet fission material, tetracene, and a PEDOT:PSS hole extraction layer. Tetracene and n-type crystalline silicon meet in a direct organic–inorganic heterojunction. In this concept the tetracene layer selectively absorbs blue-green light, generating triplet pairs that can dissociate or resonantly transfer at the organo-silicon interface, while lower-energy light is transmitted to the silicon absorber. UV photoemission measurements of the organic–inorganic interface showed an energy level alignment conducive to selective hole extraction from silicon by the organic layer. This was borne out by current–voltage measurements of devices subsequently produced. In these devices, the silicon substrate remained well-passivated beneath the tetracene thin film. Light absorption in the tetracene layer created a net reduction in current for the solar cell, but optical modelling of the external quantum efficiency spectrum suggested a small photocurrent contribution from the layer. This is a promising first result for the direct heterojunction approach to singlet fission on crystalline silicon.

Liquid phase crystallized silicon thin film solar cells on glass provide efficiencies up to 14.2 . While open circuit voltage and fill factor are already comparable to wafer based devices, short circuit current density is reduced due to incomplete light absorption. This paper analyzes the losses of current device designs in experiment and one dimensional simulations, revealing the low absorber thickness of 15 20 amp; 956;m as well as the planar glass silicon interface as the main cause of non absorption. Interface textures, in particular a sinusoidal texture and a smooth anti reflective three dimensional SMART texture, are discussed concerning their potential to mitigate these losses, allowing to reduce losses at the glass silicon interface by at least 40 relative. Taking the electronic interface quality into account, the SMART texture is identified as the most promising texture for light management in liquid phase crystallized silicon thin film solar cells on glass

We present tailor-made imprinted nanostructures for light management in liquid phase crystallized silicon thin-film solar cells providing both, increased jsc by enhanced absorption and excellent electronic material-quality with Voc-values >640mV. All superstrate textures successfully enhance light in-coupling in 10-20µm thick liquid phase crystallized silicon thin-films. Moreover, the effect of combining imprinted textures at the front side with individually optimized light trapping schemes at the rear side of the absorber layers on the optical properties is analyzed. With a silicon absorber layer thickness of 17µm maximum achievable short-circuit current density of 37.0mA/cm2 is obtained, an increase by + 1.8mA/cm2 (or 5.1%) compared to the optimized planar reference.

Recently, liquid phase crystallization of thin silicon films has emerged as a candidate for thin-film photovoltaics. On 10 μm thin absorbers, wafer-equivalent morphologies and open-circuit voltages were reached, leading to 13.2% record efficiency. However, short-circuit current densities are still limited, mainly due to optical losses at the glass-silicon interface. While nano-structures at this interface have been shown to efficiently reduce reflection, up to now these textures caused a deterioration of electronic silicon material quality. Therefore, optical gains were mitigated due to recombination losses. Here, the SMooth Anti-Reflective Three-dimensional (SMART) texture is introduced to overcome this trade-off. By smoothing nanoimprinted SiO x nano-pillar arrays with spin-coated TiO x layers, light in-coupling into laser-crystallized silicon solar cells is significantly improved as successfully demonstrated in three-dimensional simulations and in experiment. At the same time, electronic silicon material quality is equivalent to that of planar references, allowing to reach V oc values above 630 mV. Furthermore, the short-circuit current density could be increased from 21.0 mA cm−2 for planar reference cells to 24.5 mA cm−2 on SMART textures, a relative increase of 18%. External quantum efficiency measurements yield an increase for wavelengths up to 700 nm compared to a state-of-the-art solar cell with 11.9% efficiency, corresponding to a j sc, EQE gain of 2.8 mA cm−2.