Sublimed C60 for efficient and repeatable perovskite-based solar cells.

Thermally evaporated C60 is a near-ubiquitous electron transport layer in state-of-the-art p-i-n perovskite-based solar cells. As perovskite photovoltaic technologies are moving toward industrialization, batch-to-batch reproducibility of device performances becomes crucial. Here, we show that commercial as-received (99.75% pure) C60 source materials may coalesce during repeated thermal evaporation processes, jeopardizing such reproducibility. We find that the coalescence is due to oxygen present in the initial source powder and leads to the formation of deep states within the perovskite bandgap, resulting in a systematic decrease in solar cell performance. However, further purification (through sublimation) of the C60 to 99.95% before evaporation is found to hinder coalescence, with the associated solar cell performances being fully reproducible after repeated processing. We verify the universality of this behavior on perovskite/silicon tandem solar cells by demonstrating their open-circuit voltages and fill factors to remain at 1950 mV and 81% respectively, over eight repeated processes using the same sublimed C60 source material. Notably, one of these cells achieved a certified power conversion efficiency of 30.9%. These findings provide insights crucial for the advancement of perovskite photovoltaic technologies towards scaled production with high process yield.

Pathways toward commercial perovskite/silicon tandem photovoltaics.

Perovskite/silicon tandem solar cells offer a promising route to increase the power conversion efficiency of crystalline silicon (c-Si) solar cells beyond the theoretical single-junction limitations at an affordable cost. In the past decade, progress has been made toward the fabrication of highly efficient laboratory-scale tandems through a range of vacuum- and solution-based perovskite processing technologies onto various types of c-Si bottom cells. However, to become a commercial reality, the transition from laboratory to industrial fabrication will require appropriate, scalable input materials and manufacturing processes. In addition, perovskite/silicon tandem research needs to increasingly focus on stability, reliability, throughput of cell production and characterization, cell-to-module integration, and accurate field-performance prediction and evaluation. This Review discusses these aspects in view of contemporary solar cell manufacturing, offers insights into the possible pathways toward commercial perovskite/silicon tandem photovoltaics, and highlights research opportunities to realize this goal.

Enhanced optoelectronic coupling for perovskite/silicon tandem solar cells.

Monolithic perovskite/silicon tandem solar cells are of great appeal as they promise high power conversion efficiencies (PCEs) at affordable cost. In state-of-the-art tandems, the perovskite top cell is electrically coupled to a silicon heterojunction bottom cell by means of a self-assembled monolayer (SAM), anchored on a transparent conductive oxide (TCO), which enables efficient charge transfer between the subcells1-3. Yet reproducible, high-performance tandem solar cells require energetically homogeneous SAM coverage, which remains challenging, especially on textured silicon bottom cells. Here, we resolve this issue by using ultrathin (5-nm) amorphous indium zinc oxide (IZO) as the interconnecting TCO, exploiting its high surface-potential homogeneity resulting from the absence of crystal grains and higher density of SAM anchoring sites when compared with commonly used crystalline TCOs. Combined with optical enhancements through equally thin IZO rear electrodes and improved front contact stacks, an independently certified PCE of 32.5% was obtained, which ranks among the highest for perovskite/silicon tandems. Our ultrathin transparent contact approach reduces indium consumption by approximately 80%, which is of importance to sustainable photovoltaics manufacturing4.

Efficient and stable perovskite-silicon tandem solar cells through contact displacement by MgFx.

The performance of perovskite solar cells with inverted polarity (p-i-n) is still limited by recombination at their electron extraction interface, which also lowers the power conversion efficiency (PCE) of p-i-n perovskite-silicon tandem solar cells. A MgFx interlayer with thickness of ~1 nanometer at the perovskite/C60 interface favorably adjusts the surface energy of the perovskite layer through thermal evaporation, which facilitates efficient electron extraction and displaces C60 from the perovskite surface to mitigate nonradiative recombination. These effects enable a champion open-circuit voltage of 1.92 volts, an improved fill factor of 80.7%, and an independently certified stabilized PCE of 29.3% for a monolithic perovskite-silicon tandem solar cell ~1 square centimeter in area. The tandem retained ~95% of its initial performance after damp-heat testing (85°C at 85% relative humidity) for >1000 hours.

Scaled Deposition of Ti3C2Tx MXene on Complex Surfaces: Application Assessment as Rear Electrodes for Silicon Heterojunction Solar Cells.

Two-dimensional transition metal carbides (MXenes) are of great interest as electrode materials for a variety of applications, including solar cells, due to their tunable optoelectronic properties, high metallic conductivity, and attractive solution processability. However, thus far, MXene electrodes have only been exploited for lab-scale device applications. Here, to demonstrate the potential of MXene electrodes at an industry-relevant level, we implemented a scalable spray coating technique to deposit highly conductive (ca. 8000 S/cm, at a ca. 55 nm thickness) Ti3C2Tx films (Tx: surface functional groups, i.e., -OH, -O, -F) via an automated spray system. We employed these Ti3C2Tx films as rear electrodes for silicon heterojunction solar cells as a proof of concept. The spray-deposited MXene flakes have formed a conformal coating on top of the indium tin oxide (ITO)-coated random pyramidal textured silicon wafers, leading to >20% power conversion efficiency (PCE) over both medium-sized (4.2 cm2) and large (243 cm2, i.e., industry-sized 6 in. pseudosquare wafers) cell areas. Notably, the Ti3C2Tx-rear-contacted devices have retained around 99% of their initial PCE for more than 600 days of ambient air storage. Their performance is comparable with state-of-the-art solar cells contacted with sputtered silver electrodes. Our findings demonstrate the high-throughput potential of spray-coated MXene-based electrodes for solar cells in addition to a wider variety of electronic device applications.

Coupled modelling approach for optimization of bifacial silicon heterojunction solar cells with multi-scale interface textures.

For advanced optical analysis and optimization of solar cell structures with multi-scale interface textures, we applied a coupled modelling approach (CMA), where we couple the rigorous coupled wave analysis method with ray tracing and transfer matrix method. Coupling of the methods enables accurate optical analysis of solar cells made of thin coherent and thick incoherent layers and includes combinations of nano- and micro-scale textures at various positions in the structure. The approach is experimentally validated on standalone single- and both-side textured crystalline silicon wafers, as well as on complete silicon heterojunction (Si HJ) solar cell structures. Using CMA, fully encapsulated bifacial Si HJ solar cells are optically simulated first by applying single- and both-side illumination, and the effects of introducing nano inverted pyramids and random micro-pyramids at front and/or rear interfaces are analyzed. Secondly, an external light management foil with a three-sided pyramidal micro-texture is applied in simulations to the front and/or rear encapsulation glass, and the related improvements are quantified. For the optimal combination of internal textures in the analyzed structure (random micro-pyramids at the front and nano inverted pyramids at the back) and the use of the light management foil on both sides of the device, a 5.6% gain in the short-circuit current is predicted, compared to the reference case with no light management foil and with random micro-pyramids applied to the front and rear internal interfaces.