High-Throughput Photovoltaic Screening and Spacer-Dependent Shift Current in Two-Dimensional Hybrid Perovskites

Abstract

High-throughput first-principles screening of structurally diverse two-dimensional hybrid organic-inorganic perovskites (2D HOIPs) provides a route to systematically explore their photovoltaic properties. Here, we develop a computational workflow with two distinct objectives: spectroscopic limited maximum efficiency (SLME) screening to identify materials with promising photovoltaic potential and nonlinear shift current calculations to characterize their bulk photovoltaic response. Applying this workflow to a curated dataset of experimentally reported 2D HOIPs, we identify more than 25 compounds with SLME values above 25\% and more than 25 compounds exhibiting shift current responses exceeding 10~$μ$A/V$^2$. We then focus on the Pb-I-based 2D HOIPs with $n=1$ to investigate the influence of spacer chemistry on the shift current response, revealing substantial spacer-dependent variations in both its magnitude and spectral peak position. Overall, these results highlight the potential of high-throughput first-principles calculations to accelerate the discovery of experimentally relevant 2D HOIPs with promising photovoltaic properties while revealing how organic spacer chemistry influences their nonlinear shift photocurrent response.