Ultrathin Cu(In,Ga)Se2 solar cells are a promising way to reduce costs and to increase the electrical performance of thin film solar cells. An optical lithography process that can produce sub‐micrometer contacts in a SiO2 passivation layer at the CIGS rear contact is developed in this work. Furthermore, an optimization of the patterning dimensions reveals constrains over the features sizes. High passivation areas of the rear contact are needed to passivate the CIGS interface so that high performing solar cells can be obtained. However, these dimensions should not be achieved by using long distances between the contacts as they lead to poor electrical performance due to poor carrier extraction. This study expands the choice of passivation materials already known for ultrathin solar cells and its fabrication techniques.

Currently, one of the main limitations in ultrathin Cu(In,Ga)Se2 (CIGS) solar cells are the optical losses, since the absorber layer is thinner than the light optical path. Hence, light management, including rear optical reflection and light trapping is needed. In this work we focus on increasing the rear optical reflection. For this, a novel structure based on having a metal interlayer in between the Mo rear contact and the rear passivation layer is presented. In total, eight different metallic interlayers are compared. For the whole series, the passivation layer is aluminum oxide (Al2O3). The interlayers are used to enhance the reflectivity of the rear contact and thereby increasing the amount of light reflected back into the absorber. In order to understand the effects of the interlayer in the solar cell performance both from optical and/or electrical point of view, optical simulations were performed together with fabrication and electrical measurements. Optical simulations results are compared with current density-voltage (J-V) behavior and external quantum efficiency (EQE) measurements. A detailed comparison between all the interlayers is done, in order to identify the material with the greatest potential to be used as rear reflective layer for ultrathin CIGS solar cells and to establish fabrication challenges. The Ti-W alloy is a promising rear reflective layer since it provides solar cells with light to power conversion efficiency values of 9.9 %, which is 2.2 % (abs) higher than the passivated ultrathin sample and 3.7 % (abs) higher than the unpassivated ultrathin reference sample.

Herein, it is demonstrated, by using industrial techniques, that a passivation layer with nanocontacts based on silicon oxide (SiOx) leads to significant improvements in the optoelectronical performance of ultrathin Cu(In,Ga)Se2 (CIGS) solar cells. Two approaches are applied for contact patterning of the passivation layer: point contacts and line contacts. For two CIGS growth conditions, 550 and 500 °C, the SiOx passivation layer demonstrates positive passivation properties, which are supported by electrical simulations. Such positive effects lead to an increase in the light to power conversion efficiency value of 2.6% (absolute value) for passivated devices compared with a nonpassivated reference device. Strikingly, both passivation architectures present similar efficiency values. However, there is a trade‐off between passivation effect and charge extraction, as demonstrated by the trade‐off between open‐circuit voltage (Voc) and short‐circuit current density (Jsc) compared with fill factor (FF). For the first time, a fully industrial upscalable process combining SiOx as rear passivation layer deposited by chemical vapor deposition, with photolithography for line contacts, yields promising results toward high‐performance and low‐cost ultrathin CIGS solar cells with champion devices reaching efficiency values of 12%, demonstrating the potential of SiOx as a passivation material for energy conversion devices.

One of the trends making its way through the Photovoltaics (PV) industry, is the search for new application possibilities. Cu(In,Ga)Se2 (CIGS) thin film solar cells stand out due to their class leading power conversion efficiency of 23.35 %, flexibility, and low cost. The use of sub-µm ultrathin CIGS solar cells has been gaining prevalence, due to the reduction in material consumption and the manufacturing time. Precise CIGS finite-difference time-domain (FDTD) and 3D-drift diffusion baseline models were developed for the Lumerical suite and a 1D electrical model for SCAPS, allowing for an accurate description of the optoelectronic behavior and response of thin and ultrathin CIGS solar cells. As a result, it was possible to obtain accurate descriptions of the optoelectronic behavior of thin and ultrathin solar cells, and to perform an optical study and optimization of novel light management approaches, such as, random texturization, photonic nanostructures, plasmonic nanoparticles, among others. The developed light management architectures enabled to push the optical performance of an ultrathin solar cell and even surpass the performance of a thin film solar cell, enabling a short-circuit current enhancement of 6.15 mA/cm 2 over an ultrathin reference device, without any light management integrated.

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The incorporation of interface passivation structures in ultrathin Cu(In,Ga)Se2 based solar cells is shown. The fabrication used an industry scalable lithography technique—nanoimprint lithography (NIL)—for a 15 × 15 cm2 dielectric layer patterning. Devices with a NIL nanopatterned dielectric layer are benchmarked against electron-beam lithography (EBL) patterning, using rigid substrates. The NIL patterned device shows similar performance to the EBL patterned device.The impact of the lithographic processes in the rigid solar cells’ performance were evaluated via X-ray Photoelectron Spectroscopy and through a Solar Cell Capacitance Simulator. The device on stainless-steel showed a slightly lower performance than the rigid approach, due to additional challenges of processing steel substrates, even though scanning transmission electron microscopy did not show clear evidence of impurity diffusion. Notwithstanding, time-resolved photoluminescence results strongly suggested elemental diffusion from the flexible substrate. Nevertheless, bending tests on the stainless-steel device demonstrated the mechanical stability of the CIGS-based device.

For the first time, the incorporation of interface passivation structures in ultrathin Cu(In,Ga)Se2 (CIGS) based solar cells is shown in a flexible lightweight stainless-steel substrate. The fabrication was based on an industry scalable lithography technique - nanoimprint lithography (NIL) - for a 15x15 cm2 dielectric layer patterning, needed to reduce optoelectronic losses at the rear interface. The nanopatterning schemes are usually developed by lithographic techniques or by processes with limited scalability and reproducibility (nanoparticle lift-off, spin-coating, etc). However, in this work the dielectric layer is patterned using NIL, a low cost, large area, high resolution, and high throughput technique. To assess the NIL performance, devices with a NIL nanopatterned dielectric layer are benchmarked against electron-beam lithography (EBL) patterning, using rigid substrates. Up to now, EBL is considered the most reliable technique for patterning laboratory samples. The device patterned by NIL shows similar light to power conversion efficiency average values compared to the EBL patterned device - 12.6 % vs 12.3 %, respectively - highlighting the NIL potential for application in the solar cell sector. Moreover, the impact of the lithographic processes, such as different etch by-products, in the rigid solar cells’ figures of merit were evaluated from an elemental point of view via X-ray Photoelectron Spectroscopy and electrically through a Solar Cell Capacitance Simulator (SCAPS) fitting procedure. After an optimised NIL process, the device on stainless-steel achieved an average power conversion efficiency value of 11.7 % - a slightly lower value than the one obtained for the rigid approach, due to additional challenges raised by processing and handling steel substrates, even though scanning transmission electron microscopy did not show any clear evidence of impurity diffusion towards the absorber. Notwithstanding, time-resolved photoluminescence results strongly suggested the presence of additional non-radiative recombination mechanisms in the stainless-steel absorber, which were not detected in the rigid solar cells, and are compatible with elemental diffusion from the substrate. Nevertheless, bending tests on the stainless-steel device demonstrated the mechanical stability of the CIGS-based device up to 500 bending cycles.