Dabuliene Asta, Shi Zhong-En, Leitonas Karolis, Lung Chien-Yu, Volyniuk Dmytro, Kaur Khushdeep, Matulis Vitaly, Lyakhov Dmitry, Michels Dominik, Chen Chih-Ping, Grazulevicius Juozas Vidas
Department of Polymer Chemistry and Technology, Kaunas University of Technology, Baršausko Str. 59, Kaunas LT-51423, Lithuania.
Department of Materials Engineering and Organic Electronics Research Center, Ming Chi University of Technology, New Taipei City 243, Taiwan.
ACS Appl Mater Interfaces. 2024 Jun 12;16(23):30239-30254. doi: 10.1021/acsami.4c04105. Epub 2024 May 29.
We introduce thiazolo[5,4-]thiazole (TT)-based derivatives featuring carbazole, phenothiazine, or triphenylamine donor units as hole-selective materials to enhance the performance of wide-bandgap perovskite solar cells (PSCs). The optoelectronic properties of the materials underwent thorough evaluation and were substantially fine-tuned through deliberate molecular design. Time-of-flight hole mobility TTs ranged from 4.33 × 10 to 1.63 × 10 cm V s (at an electric field of 1.6 × 10 V cm). Their ionization potentials ranged from -4.93 to -5.59 eV. Using density functional theory (DFT) calculations, it has been demonstrated that S0 → S1 transitions in TTs with carbazolyl or -butyl-phenothiazinyl substituents are characterized by local excitation (LE). Mixed intramolecular charge transfer (ICT) and LE occurred for compounds containing -butyl carbazolyl-, dimethoxy carbazolyl-, or alkoxy-substituted triphenylamino donor moieties. The selected derivatives of TT were used for the preparation of hole-selective layers (HSL) in PSC with the structure of glass/ITO/HSLs/CsFAPb(IBr)/PEAI/PCBM/BCP/Ag. The alkoxy-substituted triphenylamino containing TT () has been demonstrated to be an effective material for HSL. Its layer also functioned well as an interlayer, improving the surface of control HSL_2PACz (i.e., reducing the surface energy of 2PACz from 66.9 to 52.4 mN m), thus enabling precise control over perovskite growth energy level alignment and carrier extraction/transportation at the hole-selecting contact of PSCs. 2PACz/based devices showed an optimized performance of 19.1 and 37.0% under 1-sun and 3000 K LED (1000 lx) illuminations, respectively. These values represent improvements over those achieved by bare 2PACz-based devices, which attained efficiencies of 17.4 and 32.2%, respectively. These findings highlight the promising potential of TTs for the enhancement of the efficiencies of PSCs.
我们引入了以噻唑并[5,4 - ]噻唑（TT）为基础、具有咔唑、吩噻嗪或三苯胺供体单元的衍生物作为空穴选择性材料，以提高宽带隙钙钛矿太阳能电池（PSC）的性能。对这些材料的光电性质进行了全面评估，并通过精心的分子设计对其进行了大幅微调。飞行时间空穴迁移率TT范围为4.33×10至1.63×10厘米²伏⁻¹秒⁻¹（在电场为1.6×10⁵伏厘米⁻¹时）。它们的电离势范围为 - 4.93至 - 5.59电子伏特。使用密度泛函理论（DFT）计算表明，具有咔唑基或 - 丁基 - 吩噻嗪基取代基的TT中的S0→S1跃迁具有局域激发（LE）特征。对于含有 - 丁基咔唑基 - 、二甲氧基咔唑基 - 或烷氧基取代的三苯胺供体基团的化合物，发生了分子内混合电荷转移（ICT）和LE。所选的TT衍生物用于制备具有玻璃/ITO/空穴选择性层（HSL）/CsFAPb(IBr)/PEAI/PCBM/BCP/Ag结构的PSC中的空穴选择性层（HSL）。已证明含有烷氧基取代三苯胺的TT（）是空穴选择性层的有效材料。其层作为中间层也表现良好，改善了对照空穴选择性层2PACz的表面（即，将2PACz的表面能从66.9降低到52.4毫牛顿米⁻¹），从而能够精确控制钙钛矿生长的能级排列以及PSC空穴选择接触处的载流子提取/传输。基于2PACz/的器件在1个太阳和3000 K LED（1000勒克斯）光照下分别表现出19.1%和37.0%的优化性能。这些值比裸2PACz基器件所达到的效率分别为17.4%和32.2%有所提高。这些发现突出了TT在提高PSC效率方面的潜在前景。
