Optical Dispersion Data Analysis of Single Crystal CH3NH3PbBr3 for Optimized Perovskite Solar Cell Active Layer Absorptance

Proper derivation of CH3NH3PbX3 (CH3NH3+ = methyl ammonium or MA+; X- = Cl-, Br-, I-) optical constants is a critical step toward the development of high-performance electronic and optoelectronic perovskite devices. To date, the optical dispersion regimes at, above, and below the band gap of these materials have been inconsistently characterized by omitting or under-approximating anomalous spectral features (from ultraviolet to infrared wavelengths). In this report, we present the rigorous optical dispersion data analysis of single crystal MAPbBr3 involving variable angle spectroscopic ellipsometry data appended with transmission intensity data. This approach yields a more robust derivation of MAPbBr3 optical constants (refractive index, n, and extinction coefficient, k) for both anomalous (absorptance) and normal (no absorptance) optical dispersion regimes. Using the derived optical constants for our MAPbBr3 single crystals, illustrative modeled solar cell device designs are presented in relation to non-realistic designs prepared using representative optical constants reported in the literature to date. In comparison, our derived optical dispersion data enables the modeled design of realistic planar perovskite solar cell (PSC) optical performance where the active layer (MAPbBr3) is optimized for maximum solar radiation absorption. We further demonstrate optimized modeled planar PSC designs with minimal parasitic optical absorptance in non-active PSC device layers resulting in improved performance at broad angles of incidence (approximately 0-70°). Our robust derivation of MAPbBr3 optical properties is expected to impact the optical dispersion data analysis of all perovskite analogs and expedite targeted development of, for example, solar cell, light-emitting diode, photo and X-ray/γ-ray detector, and laser system technologies.