Theoretical study of charge-transport and optical properties of organic crystals: 4,5,9,10-pyrenedi-imides

有机晶体电荷传输和光学性质的理论研究:4,5,9,10-芘二酰亚胺

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Abstract

This work presents a systematic study of the conducting and optical properties of a family of aromatic di-imides reported recently and discusses the influences of side-chain substitution on the reorganization energies, crystal packing, electronic couplings and charge injection barrier of 4,5,9,10-pyrenedi-imide (PyDI). Quantum-chemical calculations combined with the Marcus-Hush electron transfer theory revealed that the introduction of a side chain into 4,5,9,10-pyrenedi-imide increases intermolecular steric interactions and hinders close intermolecular π-π stacking, which results in weak electronic couplings and finally causes lower intrinsic hole and electron mobility in t-C(5)-PyDI (μ(h) = 0.004 cm(2) V(-1) s(-1) and μ(e) = 0.00003 cm(2) V(-1) s(-1)) than in the C(5)-PyDI crystal (μ(h) = 0.16 cm(2) V(-1) s(-1) and μ(e) = 0.08 cm(2) V(-1) s(-1)). Furthermore, electronic spectra of C(5)-PyDI were simulated and time-dependent density functional theory calculation results showed that the predicted fluorescence maximum of t-C(5)-PyDI, corresponding to an S (1)→S (0) transition process, is located at 485 nm, which is close to the experimental value (480 nm).

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