发表机构
Humboldt-Universität zu Berlin; Institute of Materials Science, Technische Universität Darmstadt; North University of China; State Key Laboratory of Extreme Environment Optoelectronic Dynamic Measurement Technology and Instrument; Materials Genome Institute, Shanghai University; Fujian Science & Technology Innovation Laboratory for Optoelectronic Information of China（柏林洪堡大学; 达姆施塔特工业大学材料科学研究所; 中北大学; 极端环境光电动态测量技术与仪器国家重点实验室; 上海大学材料基因组研究院; 福建省光电信息科技创新实验室）
机构由 AI 辅助整理，请以论文原文为准。AI 中文总结
通过高通量第一性原理筛选二维杂化钙钛矿，识别出多种高SLME和位移电流材料，并揭示间隔基化学对位移电流响应的显著影响。
AI 中文摘要
对结构多样的二维杂化有机-无机钙钛矿（2D HOIPs）进行高通量第一性原理筛选，为系统探索其光伏性能提供了一条途径。在此，我们开发了一个具有两个不同目标的计算工作流程：光谱限制最大效率（SLME）筛选以识别具有潜在光伏应用前景的材料，以及非线性位移电流计算以表征其体光伏响应。将该工作流程应用于实验报道的2D HOIPs精选数据集，我们识别出超过25种SLME值高于25%的化合物，以及超过25种位移电流响应超过10 μA/V²的化合物。随后，我们聚焦于n=1的Pb-I基2D HOIPs，研究间隔基化学对位移电流响应的影响，揭示出其大小和光谱峰位均存在显著的间隔基依赖性变化。总体而言，这些结果凸显了高通量第一性原理计算在加速发现具有良好光伏性能且与实验相关的2D HOIPs方面的潜力，同时揭示了有机间隔基化学如何影响其非线性位移光电流响应。
英文摘要
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.
