Neha Arora

Perovskite solar cells (PSCs) with efficiencies greater than 20% have been realized only with expensive organic hole-transporting materials. We demonstrate PSCs that achieve stabilized efficiencies exceeding 20% with copper(I) thiocyanate (CuSCN) as the hole extraction layer. A fast solvent removal method enabled the creation of compact, highly conformal CuSCN layers that facilitate rapid carrier extraction and collection. The PSCs showed high thermal stability under long-term heating, although their operational stability was poor. This instability originated from potential-induced degradation of the CuSCN/Au contact. The addition of a conductive reduced graphene oxide spacer layer between CuSCN and gold allowed PSCs to retain >95% of their initial efficiency after aging at a maximum power point for 1000 hours under full solar intensity at 60°C. Under both continuous full-sun illumination and thermal stress, CuSCN-based devices surpassed the stability of spiro-OMeTAD-based PSCs.

An analytical expression has been derived for the electron and hole mobility in silicon based on both experimental data and modified Brooks-Herring theory of mobility. The resulting expression allows one to obtain electron and hole mobility as a function of concentration up to <tex xmlns:mml="http://www.w3.org/1998/Math/MathML" xmlns:xlink="http://www.w3.org/1999/xlink">\sim 10^{20}</tex> cm <sup xmlns:mml="http://www.w3.org/1998/Math/MathML" xmlns:xlink="http://www.w3.org/1999/xlink">-3</sup> in an extended and continuous temperature range (250-500 K) within ± 13 percent of the reported experimental values.

perovskite layer using pentafluorophenylethylammonium (FEA) as a fluoroarene cation inserted between the 3D light-harvesting perovskite film and the hole-transporting material (HTM). The perfluorinated benzene moiety confers an ultrahydrophobic character to the spacer layer, protecting the perovskite light-harvesting material from ambient moisture while mitigating ionic diffusion in the device. Unsealed 3D/2D PSCs retain 90% of their efficiency during photovoltaic operation for 1000 hours in humid air under simulated sunlight. Remarkably, the 2D layer also enhances interfacial hole extraction, suppressing nonradiative carrier recombination and enabling a power conversion efficiency (PCE) >22%, the highest reported for 3D/2D architectures. Our new approach provides water- and heat-resistant operationally stable PSCs with a record-level PCE.

shows a single emission peak. Furthermore, irrespective of perovskite composition, the bandgap exhibits an unusual blueshift by raising the temperature from 15 to 300 K. Density functional theory and classical molecular dynamics simulations allow for assigning the additional photoluminescence peak to the presence of molecularly disordered orthorhombic domains and also rationalize that the unusual blueshift of the bandgap with increasing temperature is due to the stabilization of the valence band maximum. Our findings provide new insights into the salient emission properties of perovskite materials, which define their performance in solar cells and light-emitting devices.