Publication date: 17th February 2025
Among the all-inorganic metal halide perovskites, mixed-halide perovskites yield superior photovoltaic parameters.[1] In all-inorganic mixed-halide perovskites, it is thereby plausible that a distortion in the octahedral framework may induce electrical polarization in the compounds and prompt high efficiency in solar cells based on them. In numerous reports, different additives were added to the active layer that enhanced the efficiency of the CsPbI3-based solar cells.[2,3] It remains to be studied if the additives unintentionally induced any kind of electrical polarization in the perovskites and augmented the charge separation upon illumination. We have considered the archetypical cesium lead triiodide series CsPbI2Br and CsPbIBr2, with the black-phase of CsPbI3 and CsPbBr3 being the end-members which with the addition of suitable additives, yielded high PCEs.[4,5] All the perovskite thin-films were formed through the conventional spin-coating process inside the glovebox on the ITO substrate. The formation of sandwiched (p-i-n) structures of the devices was completed with the thermal evaporation of 100 nm-thick aluminum strips as the top electrode. In the mixed-halide perovskites, along with the additive-induced films, a net electrical-polarization may have occurred due to the change in bond length and consequent twist in the structural parameters exhibiting amplitude-voltage butterfly loops upon polarization switching. Apart from employing piezoresponse force microscopy to investigate the ferroelectric properties, we have shown that the Kelvin probe force microscopy, after applying suitable biases to pole the materials, can also be considered to probe the electrical polarization of thin films. The role of electrical-polarization in augmenting the charge separation in the compounds and the solar cell parameters have finally been correlated; mixed-halide perovskites and additive-induced films have evidenced a piezoelectric modulus (d33), and the devices based on them yielded better solar cell parameters, as compared to those with the pristine compounds.
S.M acknowledges INSPIRE Fellowship (IF 210231) funded by Department of Science & Technology, Govt. of India.