Investigating the Photovoltaic Performance in ABO₃ Structures via the Nonlinear Bond Model for an Arbitrary Incoming...

ABO₃ structures commonly known as perovskite are of high importance in advanced material science due to their interesting optical properties. Applications range from tunable band gaps, high absorption coefficients, and versatile electronic properties, making them ideal for solar cells to light-emitting diodes and even photodetectors. In this work, we present, for the first time, a nonlinear phenomenological bond model analysis of second harmonic generation (SHG) in tetragonal ABO₃ with arbitrary input light polarization. We study the material symmetry and explore the strength of the nonlinear generalized third-rank tensorial elements, which can be exploited to produce a high SHG response if the incoming light polarization is correctly selected. We found that the calculated SHG intensity profile aligns well with existing experimental data. Additionally, as the incoming light polarization varies, we observed a smooth shift in the SHG intensity peak along with changes in the number of peaks. These observations confirm the results from existing rotational anisotropy SHG experiments. In addition, we show how spatial dispersion can contribute to the total SHG intensity. Our work highlights the possibility of studying relatively complex structures, such as ABO₃, with minimal fitting parameters due to the power of the effective bond vector structure, enabling the introduction of an effective SHG hyperpolarizability rather than a full evaluation of the irreducible SHG tensor by group theoretical analysis. Such a simplification may well lead to a better understanding of the nonlinear properties in these classes of material and, in turn, can improve our understanding of the photovoltaic performance in ABO₃ structures.