Metal effect boosts the photoelectric properties of two-dimentional Dion-Jacobson (3AMPY)(MA)3M4I13 perovskites

Abstract

Two-Dimentional (2D) Dion-Jacobson (DJ) perovskites are emerging photovoltaic materials due to their excellent rigid structures and improved environmental stability compared to 2D Ruddlesden-Popper (RP) perovskites. Herein, we adopt 3-(aminomethyl)pyridine (3AMPY) as the divalent interlayer spacer to alleviate the toxicity of lead and explore more highly potential DJ alternatives, the optoelectronic and photovoltaic performance of lead-free DJ (3AMPY)(MA)₃M₄I₁₃ perovskites are investigated by first-principles calculations, where the central metals are considered as Ba, Cd, Cu, Ge, Mg, Mn, Ni, Sn and Zn to replace Pb. Our findings reveal that introducing Mn, Cd, Ni, and Ge can effectively tune the bandgap within the optimal range of 0.90–1.60 eV for solar cell application. Notably, (3AMPY)(MA)₃Ni₄I₁₃ exhibits the most favorable optical response capacity, with the light-harvesting efficiency maintaining 80 % in the UV–Vis range. (3AMPY)(MA)₃Ge₄I₁₃ displays the most excellent carrier transport with electron mobility as high as 555.43 cm² V⁻¹ s⁻¹, exhibiting a great advantage over 2D perovskites. The predicted photovoltaic performance shows that (3AMPY)(MA)₃Mg₄I₁₃ possesses the largest open circuit voltage (V_OC) (2.12 V), (3AMPY)(MA)₃Ge₄I₁₃ has the highest short circuit current density (J_sc) (38.90 mA/cm²), and (3AMPY)(MA)₃Mn₄I₁₃ is with the highest power conversion efficiency (PCE) of 22.55 %. The metal substitutions with Cd, Ni, and Ge show promoted photovoltaic potential over (3AMPY)(MA)₃Pb₄I₁₃. These results form a basis for broadening the potential candidates of this 2D DJ series in photovoltaic perovskite solar cells (PSCs).