Photocurrent interference spectroscopy of solids and characterization of semiconductor solar-cell materials

Abstract

Photocurrent measurements are widely used to study the intrinsic optoelectronic properties of semiconductors, such as photocarrier generation efficiency and carrier mobility, as well as evaluate the performance of optoelectronic devices, such as solar cells and photodetectors. Interferometric spectroscopy precisely measures optical properties and gathers optical spectra information on semiconductors. Consequently, photocurrent-based interferometric measurements, with high signal-to-noise ratios, high resolution, and broad frequency bandwidths, can probe the energy distributions of low-density defects and impurities and investigate charge transport in materials and devices. Here, we demonstrate that photocurrent interference spectroscopy reveals the intrinsic properties of solar-cell materials: bulk crystals of GaAs and halide perovskite, and thin films of halide perovskite and quantum dot. We show that homodyne interference spectroscopy of photocurrent can monitor low-density localized states in semiconductors and that it can be used in combination with other spectroscopy techniques, such as photoluminescence measurements, to provide a deep understanding of photocurrent generation processes. Furthermore, we show that heterodyne interference spectroscopy of photocurrent can be used to investigate the frequency dependence of material parameters, such as the dielectric constant, absorption coefficient, and reflectance. As an application, we used interference spectroscopy of photocurrent to show the impact of multiexcitons on the photoabsorption and photocarrier generation processes in quantum dot solar cells. Finally, we used it to reveal the distinctive spectral characteristics at the band edge of a halide perovskite, which is considered to be an exceptional solar-cell material with high energy conversion efficiency.