新型四元硫族化合物光伏特性的高通量筛选和第一性原理研究  

Photovoltaic properties of novel quaternary chalcogenides based on high-throughput screening and first-principles calculations

作　　者：康家兴 严全河 曹浩宇 孟威威 徐飞 洪峰[1] Kang Jia-Xing;Yan Quan-He;Cao Hao-Yu;Meng Wei-Wei;Xu Fei;Hong Feng(Shanghai Key Laboratory of High Temperature Superconductors,College of Sciences,Shanghai University,Shanghai 200444,China;South China Academy of Advanced Optoelectronics,South China Normal University,Guangzhou 510006,China;State Key Laboratory of Surface Physics,Department of Physics,Fudan University,Shanghai 200433,China)

机构地区：[1]上海大学理学院,上海市高温超导重点实验室,上海200444 [2]华南师范大学,华南先进光电子研究院,广州510006 [3]复旦大学物理系,应用表面物理国家重点实验室,上海200433

出　　处：《物理学报》2024年第17期75-84,共10页Acta Physica Sinica

基　　金：国家自然科学基金(批准号:62350054,12175131,12374379)资助的课题.

摘　　要：本工作提出了一种对Cu_(2)ZnSnS_(4)中Zn元素异价取代策略,探讨了新型四元硫族化合物A_(2)M_(2)M'Q_(4)(A=Na,K,Rb,Cs,In,Tl;M=Cu,Ag,Au;M'=Ti,Zr,Hf,Ge,Sn;Q=S,Se,Te)作为新型太阳能电池吸收层材料的应用潜力.利用第一性原理高通量计算,评估了1350种A_(2)M_(2)M'Q_(4)化合物热力学稳定性、带隙、光谱极限最大效率和声子色散谱等特性.结果表明,有10种热力学和动力学稳定的候选材料,它们表现出合适的带隙,并展现出高的光吸收性能,光谱极限最大效率的理论值均超过30%.它们的电子结构和光学性质类似于Cu_(2)ZnSnS_(4),有望应用于高效单结薄膜太阳能电池.本文数据集可在https://www.doi.org/10.57760/sciencedb.j00213.00006中访问获取.In recent decades,the demand for clean energy has promoted extensive research on solar cells as a key renewable energy source.Among the various emerging absorber layer materials,Kesterite-type semiconductors have aroused significant interest.Especially,Kesterite Cu_(2)ZnSnS_(4)(CZTS)stands out as a promising candidate for low-cost thin-film solar cells due to its direct bandgap,high optical absorption coefficient,suitable bandgap(1.39–1.52 eV),and abundance of constituent elements.However,the power conversion efficiency(PCE)of CZTS-based solar cells currently lags behind that of Cu(In,Ga)Se_(2)(CIGS)cells,mainly due to insufficient opencircuit voltage caused by a large number of disordered cations and defect clusters,resulting in non-radiative recombination and band-tail states.To address these challenges,partial or complete cation substitution has become a viable strategy for altering the harmful defects in CZTS.This study proposes a heterovalent substitution of Zn in CZTS and explores the potential of novel quaternary chalcogenide compound A_(2)M_(2)M'Q_(4)(A=Na,K,Rb,Cs,In,Tl;M=Cu,Ag,Au;M'=Ti,Zr,Hf,Ge,Sn;Q=S,Se,Te)as absorbers for solar cells.By substituting elements in five prototype structures,a comprehensive material database comprising 1350 A_(2)M_(2)M'Q_(4) compounds is established.High-throughput screening and first-principles calculations are used to evaluate the thermodynamic stabilities,band gaps,spectroscopic limited maximum efficiencies(SLMEs),and phonon dispersions of these compounds.Our research results indicate that 543 compounds exhibit thermodynamic stability(E_(hull)<0.01 eV/atom),202 compounds possess suitable band gaps(1.0–1.5 eV),and 10 compounds meet all the criteria for thermodynamic and dynamic stability,suitable band gaps,and high optical absorption performance(10^(4)–10^(6) cm^(-1)),with theoretical SLME values exceeding 30%.Notably,Ibam-Rb_(2)Ag_(2)GeTe_(4) exhibits the highest SLME(31.8%)in these candidates,featuring a band gap of 1.27 eV and a small carrier effective mass(<m_(0

关 键 词：第一性原理 高通量筛选 四元硫族化合物 光伏应用 

分 类 号：TB34[一般工业技术—材料科学与工程] O469[理学—凝聚态物理] TM914.4[理学—电子物理学]