Revisiting the Charge-Transfer States at Pentacene/C60Interfaces with the GW/Bethe-Salpeter Equation Approach

被引:1
作者
Fujita, Takatoshi [1 ]
Noguchi, Yoshifumi [2 ]
Hoshi, Takeo [3 ]
机构
[1] Inst Mol Sci, Okazaki, Aichi 4440865, Japan
[2] Shizuoka Univ, Grad Sch Engn, Dept Appl Chem & Biochem Engn, Hamamatsu, Shizuoka 4328561, Japan
[3] Tottori Univ, Dept Appl Math & Phys, Tottori 6808550, Japan
基金
日本学术振兴会;
关键词
charge-transfer states; donor; acceptor interfaces; organic photovoltaics; excited-state calculations; fragment molecular orbital method; GW plus Bethe-Salpeter equation; MOLECULAR-ORBITAL CALCULATIONS; DENSITY-FUNCTIONAL THEORY; ORGANIC SOLAR-CELLS; EXCITATION-ENERGIES; ELECTRON; SEPARATION; DELOCALIZATION; INTERFACES; ENERGETICS; IMPACT;
D O I
10.3390/ma13122728
中图分类号
O64 [物理化学(理论化学)、化学物理学];
学科分类号
070304 ; 081704 ;
摘要
Molecular orientations and interfacial morphologies have critical effects on the electronic states of donor/acceptor interfaces and thus on the performance of organic photovoltaic devices. In this study, we explore the energy levels and charge-transfer states at the organic donor/acceptor interfaces on the basis of the fragment-based GW and Bethe-Salpeter equation approach. The face-on and edge-on orientations of pentacene/C(60)bilayer heterojunctions have employed as model systems. GW+Bethe-Salpeter equation calculations were performed for the local interface structures in the face-on and edge-on bilayer heterojunctions, which contain approximately 2000 atoms. Calculated energy levels and charge-transfer state absorption spectra are in reasonable agreements with those obtained from experimental measurements. We found that the dependence of the energy levels on interfacial morphology is predominantly determined by the electrostatic contribution of polarization energy, while the effects of induction contribution in the edge-on interface are similar to those in the face-on. Moreover, the delocalized charge-transfer states contribute to the main absorption peak in the edge-on interface, while the face-on interface features relatively localized charge-transfer states in the main absorption peak. The impact of the interfacial morphologies on the polarization and charge delocalization effects is analyzed in detail.
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页数:15
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