CH(3)NH(3)PbI(3) perovskite / silicon tandem solar cells: characterization based optical simulations.

In this study we analyze and discuss the optical properties of various tandem architectures: mechanically stacked (four-terminal) and monolithically integrated (two-terminal) tandem devices, consisting of a methyl ammonium lead triiodide (CH(3)NH(3)PbI(3)) perovskite top solar cell and a crystalline silicon bottom solar cell. We provide layer thickness optimization guidelines and give estimates of the maximum tandem efficiencies based on state-of-the-art sub cells. We use experimental complex refractive index spectra for all involved materials as input data for an in-house developed optical simulator CROWM. Our characterization based simulations forecast that with optimized layer thicknesses the four-terminal configuration enables efficiencies over 30%, well above the current single-junction crystalline silicon cell record of 25.6%. Efficiencies over 30% can also be achieved with a two-terminal monolithic integration of the sub-cells, combined with proper selection of layer thicknesses.

Organic-inorganic halide perovskite/crystalline silicon four-terminal tandem solar cells.

Tandem solar cells constructed from a crystalline silicon (c-Si) bottom cell and a low-cost top cell offer a promising way to ensure long-term price reductions of photovoltaic modules. We present a four-terminal tandem solar cell consisting of a methyl ammonium lead triiodide (CH3NH3PbI3) top cell and a c-Si heterojunction bottom cell. The CH3NH3PbI3 top cell exhibits broad-band transparency owing to its design free of metallic components and yields a transmittance of >55% in the near-infrared spectral region. This allows the generation of a short-circuit current density of 13.7 mA cm(-2) in the bottom cell. The four-terminal tandem solar cell yields an efficiency of 13.4% (top cell: 6.2%, bottom cell: 7.2%), which is a gain of 1.8%abs with respect to the reference single-junction CH3NH3PbI3 solar cell with metal back contact. We employ the four-terminal tandem solar cell for a detailed investigation of the optical losses and to derive guidelines for further efficiency improvements. Based on a power loss analysis, we estimate that tandem efficiencies of ∼28% are attainable using an optically optimized system based on current technology, whereas a fully optimized, ultimate device with matched current could yield up to 31.6%.

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.

Photocurrent Spectroscopy of Perovskite Layers and Solar Cells: A Sensitive Probe of Material Degradation.

Optical absorptance spectroscopy of polycrystalline CH3NH3PbI3 films usually indicates the presence of a PbI2 phase, either as a preparation residue or due to film degradation, but gives no insight on how this may affect electrical properties. Here, we apply photocurrent spectroscopy to both perovskite solar cells and coplanar-contacted layers at various stages of degradation. In both cases, we find that the presence of a PbI2 phase restricts charge-carrier transport, suggesting that PbI2 encapsulates CH3NH3PbI3 grains. We also find that PbI2 injects holes into the CH3NH3PbI3 grains, increasing the apparent photosensitivity of PbI2. This phenomenon, known as modulation doping, is absent in the photocurrent spectra of solar cells, where holes and electrons have to be collected in pairs. This interpretation provides insights into the photogeneration and carrier transport in dual-phase perovskites.

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.

Raman Spectroscopy of Organic-Inorganic Halide Perovskites.

Micro-Raman spectroscopy provides laterally resolved microstructural information for a broad range of materials. In this Letter, we apply this technique to tri-iodide (CH3NH3PbI3), tribromide (CH3NH3PbBr3), and mixed iodide-bromide (CH3NH3PbI3-xBrx) organic-inorganic halide perovskite thin films and discuss necessary conditions to obtain reliable data. We explain how to measure Raman spectra of pristine CH3NH3PbI3 layers and discuss the distinct Raman bands that develop during moisture-induced degradation. We also prove unambiguously that the final degradation products contain pure PbI2. Moreover, we describe CH3NH3PbI3-xBrx Raman spectra and discuss how the perovskite crystallographic symmetries affect the Raman band intensities and spectral shapes. On the basis of the dependence of the Raman shift on the iodide-to-bromide ratio, we show that Raman spectroscopy is a fast and nondestructive method for the evaluation of the relative iodide-to-bromide ratio.

Complex Refractive Index Spectra of CH3NH3PbI3 Perovskite Thin Films Determined by Spectroscopic Ellipsometry and Spectrophotometry.

The complex refractive index (dielectric function) of planar CH3NH3PbI3 thin films at room temperature is investigated by variable angle spectroscopic ellipsometry and spectrophotometry. Knowledge of the complex refractive index is essential for designing photonic devices based on CH3NH3PbI3 thin films such as solar cells, light-emitting diodes, or lasers. Because the directly measured quantities (reflectance, transmittance, and ellipsometric spectra) are inherently affected by multiple reflections, the complex refractive index has to be determined indirectly by fitting a model dielectric function to the experimental spectra. We model the dielectric function according to the Forouhi-Bloomer formulation with oscillators positioned at 1.597, 2.418, and 3.392 eV and achieve excellent agreement with the experimental spectra. Our results agree well with previously reported data of the absorption coefficient and are consistent with Kramers-Kronig transformations. The real part of the refractive index assumes a value of 2.611 at 633 nm, implying that CH3NH3PbI3-based solar cells are ideally suited for the top cell in monolithic silicon-based tandem solar cells.

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.