In Situ Reflectometry and Diffraction Investigation of the Multiscale Structure of p-Type Polysilicon Passivating Contacts for c-Si Solar Cells.

The integration of passivating contacts based on a highly doped polycrystalline silicon (poly-Si) layer on top of a thin silicon oxide (SiOx) layer has been identified as the next step to further increase the conversion efficiency of current mainstream crystalline silicon (c-Si) solar cells. However, the interrelation between the final properties of poly-Si/SiOx contacts and their fabrication process has not yet been fully unraveled, which is mostly due to the challenge of characterizing thin-film stacks with features in the nanometric range. Here, we apply in situ X-ray reflectometry and diffraction to investigate the multiscale (1 Å-100 nm) structural evolution of poly-Si contacts during annealing up to 900 °C. This allows us to quantify the densification and thinning of the poly-Si layer during annealing as well as to monitor the disruption of the thin SiOx layer at high temperature >800 °C. Moreover, results obtained on a broader range of thermal profiles, including firing with dwell times of a few seconds, emphasize the impact of high thermal budgets on poly-Si contacts' final properties and thus the importance of ensuring a good control of such high-temperature processes when fabricating c-Si solar cells integrating such passivating contacts. Overall, this study demonstrates the robustness of combining different X-ray elastic scattering techniques (here XRR and GIXRD), which present the unique advantage of being rapid, nondestructive, and applicable on a large sample area, to unravel the multiscale structural evolution of poly-Si contacts in situ during high-temperature processes.

Nanoscale Study of the Hole-Selective Passivating Contacts with High Thermal Budget Using C-AFM Tomography.

We investigate hole-selective passivating contacts that consist of an interfacial layer of silicon oxide (SiOx) and a layer of boron-doped SiCx(p). The fabrication process of these contacts involves an annealing step at temperatures above 750 °C which crystallizes the initially amorphous layer and diffuses dopants across the interfacial oxide into the wafer to facilitate charge transport, but it can also disrupt the SiOx layer necessary for wafer-surface passivation. To investigate the transport mechanism of the charge carriers through the selective contact and its changes during the annealing process, we utilize various characterization methods, such as transmission electron microscopy, micro Raman spectroscopy, and conductive atomic force microscopy. Combining the latter with a sequential removal of material, we assemble a tomographic reconstruction of the crystallized layer that reveals the presence of preferential vertical transport channels.

Silicon-Rich Silicon Carbide Hole-Selective Rear Contacts for Crystalline-Silicon-Based Solar Cells.

The use of passivating contacts compatible with typical homojunction thermal processes is one of the most promising approaches to realizing high-efficiency silicon solar cells. In this work, we investigate an alternative rear-passivating contact targeting facile implementation to industrial p-type solar cells. The contact structure consists of a chemically grown thin silicon oxide layer, which is capped with a boron-doped silicon-rich silicon carbide [SiCx(p)] layer and then annealed at 800-900 °C. Transmission electron microscopy reveals that the thin chemical oxide layer disappears upon thermal annealing up to 900 °C, leading to degraded surface passivation. We interpret this in terms of a chemical reaction between carbon atoms in the SiCx(p) layer and the adjacent chemical oxide layer. To prevent this reaction, an intrinsic silicon interlayer was introduced between the chemical oxide and the SiCx(p) layer. We show that this intrinsic silicon interlayer is beneficial for surface passivation. Optimized passivation is obtained with a 10-nm-thick intrinsic silicon interlayer, yielding an emitter saturation current density of 17 fA cm-2 on p-type wafers, which translates into an implied open-circuit voltage of 708 mV. The potential of the developed contact at the rear side is further investigated by realizing a proof-of-concept hybrid solar cell, featuring a heterojunction front-side contact made of intrinsic amorphous silicon and phosphorus-doped amorphous silicon. Even though the presented cells are limited by front-side reflection and front-side parasitic absorption, the obtained cell with a Voc of 694.7 mV, a FF of 79.1%, and an efficiency of 20.44% demonstrates the potential of the p+/p-wafer full-side-passivated rear-side scheme shown here.

Light trapping in solar cells: numerical modeling with measured surface textures.

We present and experimentally validate a computational model for the light propagation in thin-film solar cells that integrates non-paraxial scalar diffraction theory with non-sequential ray-tracing. The model allows computing the spectral layer absorbances of solar cells with micro- and nano-textured interfaces directly from measured surface topographies. We can thus quantify decisive quantities such as the parasitic absorption without relying on heuristic scattering intensity distributions. In particular, we find that the commonly used approximation of Lambertian scattering intensity distributions for internal light propagation is violated even for solar cells on rough textured substrates. More importantly, we demonstrate how both scattering and parasitic absorption must be controlled to maximize photocurrent.

Self-patterned nanoparticle layers for vertical interconnects: application in tandem solar cells.

We demonstrate self-patterned insulating nanoparticle layers to define local electrical interconnects in thin-film electronic devices. We show this with thin-film silicon tandem solar cells, where we introduce between the two component cells a solution-processed SiO2 nanoparticle layer with local openings to allow for charge transport. Because of its low refractive index, high transparency, and smooth surface, the SiO2 nanoparticle layer acts as an excellent intermediate reflector allowing for efficient light management.

Organometallic Halide Perovskites: Sharp Optical Absorption Edge and Its Relation to Photovoltaic Performance.

Solar cells based on organometallic halide perovskite absorber layers are emerging as a high-performance photovoltaic technology. Using highly sensitive photothermal deflection and photocurrent spectroscopy, we measure the absorption spectrum of CH3NH3PbI3 perovskite thin films at room temperature. We find a high absorption coefficient with particularly sharp onset. Below the bandgap, the absorption is exponential over more than four decades with an Urbach energy as small as 15 meV, which suggests a well-ordered microstructure. No deep states are found down to the detection limit of ∼1 cm(-1). These results confirm the excellent electronic properties of perovskite thin films, enabling the very high open-circuit voltages reported for perovskite solar cells. Following intentional moisture ingress, we find that the absorption at photon energies below 2.4 eV is strongly reduced, pointing to a compositional change of the material.

Plasmonic silicon solar cells: impact of material quality and geometry.

We study n-i-p amorphous silicon solar cells with light-scattering nanoparticles in the back reflector. In one configuration, the particles are fully embedded in the zinc oxide buffer layer; In a second configuration, the particles are placed between the buffer layer and the flat back electrode. We use stencil lithography to produce the same periodic arrangement of the particles and we use the same solar cell structure on top, thus establishing a fair comparison between a novel plasmonic concept and its more traditional counterpart. Both approaches show strong resonances around 700 nm in the external quantum efficiency the position and intensity of which vary strongly with the nanoparticle shape. Moreover, disagreement between simulations and our experimental results suggests that the dielectric data of bulk silver do not correctly represent the reality. A better fit is obtained by introducing a porous interfacial layer between the silver and zinc oxide. Without the interfacial layer, e.g. by improved processing of the nanoparticles, our simulations show that the nanoparticles concept could outperform traditional back reflectors.

Nanomoulding of functional materials, a versatile complementary pattern replication method to nanoimprinting.

We describe a nanomoulding technique which allows low-cost nanoscale patterning of functional materials, materials stacks and full devices. Nanomoulding combined with layer transfer enables the replication of arbitrary surface patterns from a master structure onto the functional material. Nanomoulding can be performed on any nanoimprinting setup and can be applied to a wide range of materials and deposition processes. In particular we demonstrate the fabrication of patterned transparent zinc oxide electrodes for light trapping applications in solar cells.

Light trapping in solar cells: can periodic beat random?

Theory predicts that periodic photonic nanostructures should outperform their random counterparts in trapping light in solar cells. However, the current certified world-record conversion efficiency for amorphous silicon thin-film solar cells, which strongly rely on light trapping, was achieved on the random pyramidal morphology of transparent zinc oxide electrodes. Based on insights from waveguide theory, we develop tailored periodic arrays of nanocavities on glass fabricated by nanosphere lithography, which enable a cell with a remarkable short-circuit current density of 17.1 mA/cm(2) and a high initial efficiency of 10.9%. A direct comparison with a cell deposited on the random pyramidal morphology of state-of-the-art zinc oxide electrodes, replicated onto glass using nanoimprint lithography, demonstrates unambiguously that periodic structures rival random textures.

Nanoimprint lithography for high-efficiency thin-film silicon solar cells.

We demonstrate high-efficiency thin-film silicon solar cells with transparent nanotextured front electrodes fabricated via ultraviolet nanoimprint lithography on glass substrates. By replicating the morphology of state-of-the-art nanotextured zinc oxide front electrodes known for their exceptional light trapping properties, conversion efficiencies of up to 12.0% are achieved for micromorph tandem junction cells. Excellent light incoupling results in a remarkable summed short-circuit current density of 25.9 mA/cm(2) for amorphous top cell and microcrystalline bottom cell thicknesses of only 250 and 1100 nm, respectively. As efforts to maximize light harvesting continue, our study validates nanoimprinting as a versatile tool to investigate nanophotonic effects of a large variety of nanostructures directly on device performance.

Understanding of photocurrent enhancement in real thin film solar cells: towards optimal one-dimensional gratings.

Despite the progress in the engineering of structures to enhance photocurrent in thin film solar cells, there are few comprehensive studies which provide general and intuitive insight into the problem of light trapping. Also, lack of theoretical propositions which are consistent with fabrication is an issue to be improved. We investigate a real thin film solar cell with almost conformal layers grown on a 1D grating metallic back-reflector both experimentally and theoretically. Photocurrent increase is observed as an outcome of guided mode excitation in both theory and experiment by obtaining the external quantum efficiency of the cell for different angles of incidence and in both polarization directions. Finally, the effect of geometrical parameters on the short circuit current density of the device is investigated by considering different substrate shapes that are compatible with solar cell fabrication. Based on our simulations, among the investigated shapes, triangular gratings with a very sharp slope in one side, so called sawtooth gratings, are the most promising 1D gratings for optimal light trapping.

Surface chirality of CuO thin films.

We present X-ray photoelectron spectroscopy (XPS) and X-ray photoelectron diffraction (XPD) investigations of CuO thin films electrochemically deposited on an Au(001) single-crystal surface from a solution containing chiral tartaric acid (TA). The presence of enantiopure TA in the deposition process results in a homochiral CuO surface, as revealed by XPD. On the other hand, XPD patterns of films deposited with racemic tartaric acid or the "achiral" meso-tartaric acid are completely symmetric. A detailed analysis of the experimental data using single scattering cluster calculations reveals that the films grown with l(+)-TA exhibit a CuO(1) orientation, whereas growth in the presence of d(-)-TA results in a CuO(11) surface orientation. A simple bulk-truncated model structure with two terminating oxygen layers reproduces the experimental XPD data. Deposition with alternating enantiomers of tartaric acid leads to CuO films of alternating chirality. Enantiospecifity of the chiral CuO surfaces is demonstrated by further deposition of CuO from a solution containing racemic tartaric acid. The pre-deposited homochiral films exhibit selectivity toward the same enantiomeric deposition pathway.