材料科学
发色团
阳离子聚合
太赫兹辐射
光电子学
班级(哲学)
非线性光学
光学
纳米技术
光化学
高分子化学
物理
激光器
化学
人工智能
计算机科学
作者
Jeong‐A Yang,Chae‐Won Lee,Chaeyoon Kim,Michael Auer,In Cheol Yu,Je Hoon Oh,Woojin Yoon,Hoseop Yun,Dongwook Kim,Mojca Jazbinšek,Fabıan Rotermund,O‐Pil Kwon
标识
DOI:10.1002/adom.202400343
摘要
Abstract A strategic approach to develop efficient ultra‐broadband terahertz (THz) crystals involves the incorporation of different electron donating groups (EDGs) into cationic chromophores. In contrast to the widely utilized non‐cyclic 4‐(dimethylamino)phenyl (DA) EDG, cyclic 5‐membered 4‐(2‐(hydroxymethyl)pyrrolidine‐1‐yl)phenyl (PB) and cyclic 6‐membered 4‐(3‐(hydroxymethyl)piperidin‐1‐yl)phenyl (PN) EDGs exhibit an asymmetrical shape with a strongly interacting hydroxymethyl group at the chiral center. Notably, the PB EDG shows narrower intrinsic vibrational states with lower conformational flexibility and smaller ring flips compared to the PN EDG. In the crystalline state, introducing the PB EDG leads to the formation of a new class of nonlinear optical assembly, the so‐called stair‐type cation‐anion assembly. This assembly demonstrates optimal chromophore alignment with state‐of‐the‐art effective first hyperpolarizability (209 × 10 −30 esu). Furthermore, the PB EDG‐based crystals exhibit significantly lower THz absorption compared to previously reported benchmark crystals. In THz wave generation experiments, PB EDG‐based crystals demonstrate state‐of‐the‐art efficiency and ultrabroad spectral bandwidth, featuring a cut‐off frequency of up to 16 THz.
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