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Tuning Solid-State Luminescence in Conjugated Organic Materials: Control of Excitonic and Excimeric Contributions through π Stacking and Halogen Bond Driven Self-Assembly.
ChemPhysChem ( IF 2.3 ) Pub Date : 2020-02-14 , DOI: 10.1002/cphc.201901223 Prabhat Majumdar 1 , Fazil Tharammal 1 , Johannes Gierschner 2 , Shinto Varghese 1
ChemPhysChem ( IF 2.3 ) Pub Date : 2020-02-14 , DOI: 10.1002/cphc.201901223 Prabhat Majumdar 1 , Fazil Tharammal 1 , Johannes Gierschner 2 , Shinto Varghese 1
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Two polymorphs with distinctly different fluorescence emission (green and yellow; G, Y) emanating from excitonic and excimeric contributions were prepared from solution as well as by using physical vapour transport. Based on crystal structure investigations, the vibrationally‐resolved excitonic emission is found to originate from a β‐Sheet arrangement (G), whereas a sandwich herringbone structure is responsible for the excimer emission (Y). The intermolecular interactions and energies were quantified to have a complete picture of the decisive factors that controls the self‐assembly. Halogen‐bond directed self‐assembly was explored to fine‐tune the intermolecular interactions through co‐crystallization as well as a commercially viable liquid assisted grinding method. A smooth fluorescence shift from G to Y was achieved by co‐assembly due to substantial differences in the π orbital overlap in the molecular packing. Our investigation provides a comprehensive understanding of the origin of excitonic and excimeric contributions of emission behaviour in conjunction with the molecular packing and π–π orbital overlap, and might provide a directive towards the engineering of fluorescent functional molecular materials.
中文翻译：
调整共轭有机材料中的固态发光：通过π堆积和卤素键驱动的自组装控制激子和激基贡献。
由溶液和利用物理气相传输制备了两种由激子和激子贡献产生的荧光发射（绿色和黄色； G，Y）明显不同的多晶型物。根据晶体结构研究，发现振动解析的激子发射源自β-Sheet排列（G），而夹层人字形结构则是准分子发射（Y）的原因。分子间的相互作用和能量被量化以完整地掌握决定自组装的决定性因素。探索了卤素键定向自组装技术，通过共结晶以及商业上可行的液体辅助研磨方法来微调分子间的相互作用。由于分子堆积中π轨道重叠的显着差异，通过共组装实现了从G到Y的平稳荧光转换。我们的研究对分子结构和π-π轨道重叠以及分子行为和分子结构的相互作用提供了对激子和激射行为贡献的全面理解，并可能为荧光功能分子材料的工程设计提供指导。
更新日期：2020-02-14
中文翻译：
调整共轭有机材料中的固态发光：通过π堆积和卤素键驱动的自组装控制激子和激基贡献。
由溶液和利用物理气相传输制备了两种由激子和激子贡献产生的荧光发射（绿色和黄色； G，Y）明显不同的多晶型物。根据晶体结构研究，发现振动解析的激子发射源自β-Sheet排列（G），而夹层人字形结构则是准分子发射（Y）的原因。分子间的相互作用和能量被量化以完整地掌握决定自组装的决定性因素。探索了卤素键定向自组装技术，通过共结晶以及商业上可行的液体辅助研磨方法来微调分子间的相互作用。由于分子堆积中π轨道重叠的显着差异，通过共组装实现了从G到Y的平稳荧光转换。我们的研究对分子结构和π-π轨道重叠以及分子行为和分子结构的相互作用提供了对激子和激射行为贡献的全面理解，并可能为荧光功能分子材料的工程设计提供指导。
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