In recent years, the strategies used to break the Cu(In,Ga)Se2 (CIGS) world record of light to power conversion efficiency, were based on improvements of the absorber optoelectronic and crystalline properties, mainly using complex post-deposition treatments. To reach even higher efficiency values, advances in the solar cell architecture are needed focusing in the CIGS interfaces. In this study, we evaluate the structural, morphological and optoelectronic impact on the CIGS properties of using an Al2O3 layer as a potential front passivation layer. The impact of Al2O3 tunnelling layer between CIGS and CdS is also addressed in this study. Morphological and structural analyses reveal that the use of Al2O3 alone is not detrimental to CIGS, although it does not resist to the CdS chemical bath deposition. When CdS is deposited on top of Al2O3, the CIGS optoelectronic properties are heavily degraded. Nonetheless, when Al2O3 is used alone, optoelectronic measurements reveal a positive impact of its inclusion such as a very low concentration of interface defects and the CIGS keeping the same recombination channels. With the findings of this study the best use of Al2O3 front passivation layer could be with alternative buffer layers. The Al2O3 layer will keep the CIGS surface with a low density of defects while keeping its structural and optoelectronic properties as good as the ones when CdS is deposited. It can also be reported that a comparison between the different analyses allowed us to strongly suggest for the first time that low-energy muon spin spectroscopy (LE-μSR) is sensitive to both charge carrier separation and bulk recombination in complex semiconductors.

The incorporation of nanostructures in optoelectronic devices for enhancing their optical performance is widely studied. However, several problems related to the processing complexity and the low performance of the nanostructures have hindered such actions in real‐life devices. Herein, a novel way of introducing gold nanoparticles in a solar cell structure is proposed in which the nanostructures are encapsulated with a dielectric layer, shielding them from high temperatures and harsh growth processing conditions of the remaining device. Through optical simulations, an enhancement of the effective optical path length of approximately four times the nominal thickness of the absorber layer is verified with the new architecture. Furthermore, the proposed concept in a Cu(In,Ga)Se2 solar cell device is demonstrated, where the short‐circuit current density is increased by 17.4%. The novel structure presented in this work is achieved by combining a bottom‐up chemical approach of depositing the nanostructures with a top‐down photolithographic process, which allows for an electrical contact.

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.

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.

A decentralized energy system requires photovoltaic solutions to meet new aesthetic paradigms, such as lightness, flexibility, and new form factors. Notwithstanding, the materials shortage in the Green Transition is a concern gaining momentum due to their foreseen continuous demand. A fruitful strategy to shrink the absorber thickness, meeting aesthetic and shortage materials consumption targets, arises from interface passivation. However, a deep understanding of passivated systems is required to close the efficiency gap between ultra‐thin and thin film devices, and to mono‐Si. Herein, a (Ag,Cu)(In,Ga)Se2 ultra‐thin solar cell, with 92% passivated rear interface area, is compared with a conventional nonpassivated counterpart. A thin MoSe2 layer, for a quasi‐ohmic contact, is present in the two architectures at the contacts, despite the passivated device narrow line scheme. The devices present striking differences in charge carrier dynamics. Electrical and optoelectronic analysis combined with SCAPS modelling suggest a lower recombination rate for the passivated device, through a reduction on the rear surface recombination velocity and overall defects, comparing with the reference solar cell. The new architecture allows for a 2% efficiency improvement on a 640 nm ultra‐thin device, from 11% to 13%, stemming from an open circuit voltage increase of 108 mV.

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