期刊
NANO LETTERS
卷 17, 期 3, 页码 1719-1726出版社
AMER CHEMICAL SOC
DOI: 10.1021/acs.nanolett.6b04995
关键词
Merocyanine dyes; exciton coupling dipole moments; dye aggregates; supramolecular chemistry; crystal engineering
类别
资金
- Bavarian State Ministry of Science, Research, and the Arts for the Collaborative Research Network Solar Technologies go Hybrid
A key issue for the application of pi-conjugated organic molecules as thin film solid-state materials is the packing structure, which drastically affects optical and electronic properties due to intermolecular coupling. In this regard, merocyanine dyes usually pack in H-coupled antiparallel arrangements while structures with more interesting J-type coupling have been rarely reported. Here we show that for three highly dipolar merocyanine dyes, which exhibit the same it scaffold and accordingly equal properties as monomers in solution, the solid-state packing can be changed by a simple variation of aliphatic substituents to afford narrow and intense absorption bands with huge hypsochromic (H) or bathochromic (J) shifts for their thin films and nanocrystals. Time-dependent density functional theory calculations show that the energetic offset of almost 1 eV magnitude results from distinct packing motifs within the crystal structures that comply with the archetype H- or J-aggregate structures as described by Kasha's exciton theory.
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