Beijing National Laboratory for Molecular Science (BNLMS), Key Laboratory of Colloid, Interface and Chemical Thermodynamics, Institute of Chemistry, Chinese Academy of Sciences, ZhongGuanCun North First Street 2, Beijing, 100190, China.
College of Chemistry and Molecular Engineering, Zhengzhou University, Kexuedadao 100, Zhengzhou, 450001, China.
Angew Chem Int Ed Engl. 2022 Jul 18;61(29):e202205633. doi: 10.1002/anie.202205633. Epub 2022 May 19.
Here, we combined the merits of emergent excitation-dependent (ExD) emission and circularly polarized luminescence to develop an excitation-dependent circularly polarized luminescence (ExD CPL) material showing unique features. A series of acylhydrazones based on a chiral tartaric skeleton was designed and found to self-assemble into helical nanostructures through non-covalent bonds. The helical assemblies showed ExD CPL due to the cooperation of chirality transfer and excited state intramolecular proton transfer (ESIPT). Remarkably, not only the emission wavelength could be tuned by the excitation wavelength but the handedness of CPL could be modulated in an inverted or ON/OFF manner as well, thus leading to the first example of an ExD inverted or ON/OFF switchable CPL system. Time-dependent density functional theory (TD-DFT) calculations were carried out to explain the inversion of ExD CPL. This work provided a new insight into the unprecedented handedness controllable ExD CPL, which showcased a new paradigm of the advanced CPL materials.
在这里,我们结合了突发激发依赖(ExD)发射和圆偏振发光的优点,开发了一种激发依赖的圆偏振发光(ExD CPL)材料,该材料具有独特的性质。我们设计了一系列基于手性酒石酸骨架的酰腙,并发现它们通过非共价键自组装成螺旋纳米结构。由于手性转移和激发态分子内质子转移(ESIPT)的协同作用,螺旋组装体表现出 ExD CPL。值得注意的是,不仅发射波长可以通过激发波长来调节,而且圆偏振光的手性也可以以反转或开/关的方式进行调节,从而首次实现了 ExD 反转或开/关可切换的 CPL 系统。我们进行了含时密度泛函理论(TD-DFT)计算来解释 ExD CPL 的反转。这项工作为前所未有的手性可控 ExD CPL 提供了新的见解,展示了先进 CPL 材料的新范例。