Enhanced Grain Size, Photoluminescence, and Photoconversion Efficiency with Cadmium Addition during the Two-Step Growth of CH₃NH₃PbI₃

Abstract

Control over grain size and crystallinity is important for preparation of methylammonium lead iodide (MAPbI₃) solar cells. We explore the effects of using small concentrations of Cd²⁺ and unusually high concentrations of methylammonium iodide during the growth of MAPbI₃ in the two-step solution process. In addition to improved crystallinity and an enhancement in the size of the grains, time-resolved photoluminescence measurements indicated a dramatic increase in the carrier lifetime. As a result, devices constructed with the Cd-modified perovskites showed nearly a factor of 2 improvement in the power conversion efficiency (PCE) relative to similar devices prepared without Cd addition. The grains also showed a higher degree of orientation in the ⟨110⟩ direction, indicating a change in the growth mechanism, and the films were compact and smooth. We propose a Cd-modified film growth mechanism that invokes a critical role for low-dimensional Cd perovskites to explain the experimental observations.