Achiral Solvent Inversed Helical Pathway and Cosolvent Controlled Excited-State “Majority Rule” in Enantiomeric Dansulfonamide Assemblies

IF 13 2区 材料科学 Q1 CHEMISTRY, MULTIDISCIPLINARY Small Pub Date : 2024-05-11 DOI:10.1002/smll.202401954
Xin Wen, Fulin Wang, Sifan Du, Yuqian Jiang, Li Zhang, Minghua Liu
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Abstract

Achiral solvents are commonly utilized to induce the self-assembly of chiral molecules. This study demonstrates that achiral solvents can trigger helicity inversion in the assemblies of dansyl amphiphiles and control the excited-state “majority rule” in assemblies composed of pure enantiomers, through variation of the cosolvent ratio. Specifically, enantiomers of dansyl amphiphiles self-assemble into helical structures with opposite handedness in methanol (MeOH) and acetonitrile (MeCN), together with inversed circular dichroism and circularly polarized luminescence (CPL) signals. When a mixture of MeOH and MeCN is employed, the achiral cosolvents collectively affect the CPL of the assemblies in a way similar to that of “mixed enantiomers”. The dominant cosolvent governs the CPL signal. As the cosolvent composition shifts from pure MeCN to MeOH, the CPL signals undergo a significant inversion and amplification, with two maxima observed at ≈20% MeOH and 20% MeCN. This study deepens the comprehension of how achiral solvents modulate helical nanostructures and their excited-state chiroptical properties.

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对映体丹磺酰胺组装中的非手性溶剂反向螺旋途径和共溶剂控制的激发态 "多数规则
非手性溶剂通常用于诱导手性分子的自组装。本研究证明,非手性溶剂可以通过改变共溶剂的比例,在丹酰双亲化合物的集合体中引发螺旋反转,并控制由纯对映体组成的集合体中激发态的 "多数规则"。具体来说,丹酰双亲化合物的对映体在甲醇(MeOH)和乙腈(MeCN)中自组装成手性相反的螺旋结构,同时出现反向圆二色性和圆偏振发光(CPL)信号。当使用 MeOH 和 MeCN 混合物时,非手性共溶剂会以类似于 "混合对映体 "的方式共同影响组装体的 CPL。主要的共溶剂会影响 CPL 信号。随着共溶剂成分从纯 MeCN 到 MeOH 的转变,CPL 信号发生了显著的反转和放大,在 ≈20% MeOH 和 20% MeCN 时观察到两个最大值。这项研究加深了人们对非手性溶剂如何调节螺旋纳米结构及其激发态自旋特性的理解。
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来源期刊
Small
Small 工程技术-材料科学:综合
CiteScore
17.70
自引率
3.80%
发文量
1830
审稿时长
2.1 months
期刊介绍: Small serves as an exceptional platform for both experimental and theoretical studies in fundamental and applied interdisciplinary research at the nano- and microscale. The journal offers a compelling mix of peer-reviewed Research Articles, Reviews, Perspectives, and Comments. With a remarkable 2022 Journal Impact Factor of 13.3 (Journal Citation Reports from Clarivate Analytics, 2023), Small remains among the top multidisciplinary journals, covering a wide range of topics at the interface of materials science, chemistry, physics, engineering, medicine, and biology. Small's readership includes biochemists, biologists, biomedical scientists, chemists, engineers, information technologists, materials scientists, physicists, and theoreticians alike.
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