Journal
JOURNAL OF PHYSICAL CHEMISTRY LETTERS
Volume 8, Issue 6, Pages 1118-1123Publisher
AMER CHEMICAL SOC
DOI: 10.1021/acs.jpclett.7b00283
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Funding
- Bolton Fund at Lafayette College
- EXCEL Program at Lafayette College
- NSF [DMR-1505437]
- Direct For Mathematical & Physical Scien
- Division Of Materials Research [1505437] Funding Source: National Science Foundation
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We report the polarized absorption spectra of high quality, thin crystals of a perylene diimide (PDI) species with branched side chains (B2). The absorption spectrum shows exemplary polarization-dependent H-like and J-like aggregate behavior upon orthogonal excitation, with a sizable Davydov splitting (DS) of 1230 cm(-1) and peak to peak splitting of 3040 cm(-1). The experimental results are compared to theoretical calculations with remarkable agreement. The theoretical analysis of the polarized absorption spectra shows evidence of a high degree of intermolecular charge transfer, which, along with Coulombic coupling, conspires to create the unprecedented DS for this family of dye molecules. The large polarization dependence of the electronic spectra is attributed to the unique twisted crystal structure, in which a substantial rotational displacement exists between neighboring chromophores within a pi-stack. These results highlight the strong intermolecular geometry in PDI systems.
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