Publication date: 17th July 2025
Low-dimensional lead halide perovskites have gained significant attention as exceptional semiconducting materials, owing to their unique photophysical characteristics and remarkable nonlinear optical properties. Intentional doping of these low-dimensional perovskites with diverse impurities has recently attracted renewed attention, as it offers a promising route to enhance their optoelectronic performance for a wide range of practical applications.1 While they possess remarkable optoelectronic properties, the underlying nonlinear responses and charge transport mechanisms with doping are yet to be thoroughly investigated. In this work, we have substituted Pb2+ ions with isovalent Mn2+ and heterovalent Sb3+ ions in 2D layered perovskite, PEA2PbI4. Utilizing the third-harmonic generation (THG) technique, the third-order nonlinear susceptibility, optical stability, and anisotropic properties of the PEA2PbI4 were studied in the doped and undoped materials.2 The results revealed a significantly enhanced THG response on doping, attributed to defect states acting as optical transition pathways, along with a decline in optical stability, indicating potential defect-induced degradation. To gain further insight into the charge-carrier dynamics at varying doping levels, optical pump-terahertz probe (OPTP) spectroscopy was performed.3-4 The analysis revealed ultrafast free-carrier relaxation attributed to the quantum well structures inherent in the 2D perovskite. Additionally, a reduction in carrier mobility and initial photoconductivity was observed with increasing defect population introduced by doping. This understanding suggests the need to optimize the charge carrier transport for tuning the optoelectronic properties.
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