Optical modeling of wide-bandgap perovskite and perovskite/silicon tandem solar cells using complex refractive indices for arbitrary-bandgap perovskite absorbers.

Wide-bandgap perovskites are attractive top-cell materials for tandem photovoltaic applications. Comprehensive optical modeling is essential to minimize the optical losses of state-of-the-art perovskite/perovskite, perovskite/CIGS, and perovskite/silicon tandems. Such models require accurate optical constants of wide-bandgap perovskites. Here, we report optical constants determined with ellipsometry and spectrophotometry for two new wide-bandgap, cesium-formamidinium-based perovskites. We validate the optical constants by comparing simulated quantum efficiency and reflectance spectra with measured cell results for semi-transparent single-junction perovskite cells and find less than 0.3 mA/cm2 error in the short-circuit current densities. Such simulations further reveal that reflection and parasitic absorption in the front ITO layer and electron contact are responsible for the biggest optical losses. We also show that the complex refractive index of methylammonium lead triiodide, the most common perovskite absorber for solar cells, can be used to generate approximate optical constants for an arbitrary wide-bandgap perovskite by translating the data along the wavelength axis. Finally, these optical constants are used to map the short-circuit current density of a textured two-terminal perovskite/silicon tandem solar cell as a function of the perovskite thickness and bandgap, providing a guide to nearly 20 mA/cm2 matched current density with any perovskite bandgap between 1.56 and 1.68 eV.

In Situ Measurement of Electric-Field Screening in Hysteresis-Free PTAA/FA0.83Cs0.17Pb(I0.83Br0.17)3/C60 Perovskite Solar Cells Gives an Ion Mobility of ∼3 × 10-7 cm2/(V s), 2 Orders of Magnitude Faster than Reported for Metal-Oxide-Contacted Perovskite Cells with Hysteresis.

We apply a series of transient measurements to operational perovskite solar cells of the architecture ITO/PTAA/FA0.83Cs0.17Pb(I0.83Br0.17)3/C60/BCP/Ag, and similar cells with FA0.83MA0.17. The cells show no detectable JV hysteresis. Using photocurrent transients at applied bias we find a ∼1 ms time scale for the electric field screening by mobile ions in these cells. We confirm our interpretation of the transient measurements using a drift-diffusion model. Using Coulometry during field screening relaxation at short circuit, we determine the mobile ion concentration to be ∼1 × 1018/cm3. Using a model with one mobile ion species, the concentration and the screening time require an ion mobility of ∼3 × 10-7 cm2/(V s). As far as we know, this article gives the first direct measurement of the ion mobility and concentration in a fully functional perovskite solar cell. The measured ion mobility is 2 orders of magnitude higher than the highest estimates previously determined using perovskite solar cells and perovskite thin films, and 3 orders of magnitude higher than is frequently used in modeling hysteresis effects. We provide evidence that the fast field screening is due to mobile ions, as opposed to dark injection and trapping of electronic carriers.

Perovskite-perovskite tandem photovoltaics with optimized band gaps.

We demonstrate four- and two-terminal perovskite-perovskite tandem solar cells with ideally matched band gaps. We develop an infrared-absorbing 1.2-electron volt band-gap perovskite, FA0.75Cs0.25Sn0.5Pb0.5I3, that can deliver 14.8% efficiency. By combining this material with a wider-band gap FA0.83Cs0.17Pb(I0.5Br0.5)3 material, we achieve monolithic two-terminal tandem efficiencies of 17.0% with >1.65-volt open-circuit voltage. We also make mechanically stacked four-terminal tandem cells and obtain 20.3% efficiency. Notably, we find that our infrared-absorbing perovskite cells exhibit excellent thermal and atmospheric stability, not previously achieved for Sn-based perovskites. This device architecture and materials set will enable "all-perovskite" thin-film solar cells to reach the highest efficiencies in the long term at the lowest costs.

Cross-Linkable, Solvent-Resistant Fullerene Contacts for Robust and Efficient Perovskite Solar Cells with Increased JSC and VOC.

The active layers of perovskite solar cells are also structural layers and are central to ensuring that the structural integrity of the device is maintained over its operational lifetime. Our work evaluating the fracture energies of conventional and inverted solution-processed MAPbI3 perovskite solar cells has revealed that the MAPbI3 perovskite exhibits a fracture resistance of only ∼0.5 J/m2, while solar cells containing fullerene electron transport layers fracture at even lower values, below ∼0.25 J/m2. To address this weakness, a novel styrene-functionalized fullerene derivative, MPMIC60, has been developed as a replacement for the fragile PC61BM and C60 transport layers. MPMIC60 can be transformed into a solvent-resistant material through curing at 250 °C. As-deposited films of MPMIC60 exhibit a marked 10-fold enhancement in fracture resistance over PC61BM and a 14-fold enhancement over C60. Conventional-geometry perovskite solar cells utilizing cured films of MPMIC60 showed a significant, 205% improvement in fracture resistance while exhibiting only a 7% drop in PCE (13.8% vs 14.8% PCE) in comparison to the C60 control, enabling larger VOC and JSC values. Inverted cells fabricated with MPMIC60 exhibited a 438% improvement in fracture resistance with only a 6% reduction in PCE (12.3% vs 13.1%) in comparison to those utilizing PC61BM, again producing a higher JSC.

Thermal and Environmental Stability of Semi-Transparent Perovskite Solar Cells for Tandems Enabled by a Solution-Processed Nanoparticle Buffer Layer and Sputtered ITO Electrode.

A sputtered oxide layer enabled by a solution-processed oxide nanoparticle buffer layer to protect underlying layers is used to make semi-transparent perovskite solar cells. Single-junction semi-transparent cells are 12.3% efficient, and mechanically stacked tandems on silicon solar cells are 18.0% efficient. The semi-transparent perovskite solar cell has a T 80 lifetime of 124 h when operated at the maximum power point at 100 °C without additional sealing in ambient atmosphere under visible illumination.