Insight into the Origin of Trapping in Polymer/Fullerene Blends with a Systematic Alteration of the Fullerene to Higher Adducts

富勒烯 离域电子 聚合物 材料科学 化学物理 超快激光光谱学 轨道能级差 光化学 光谱学 化学 有机化学 分子 物理 量子力学 复合材料
作者
Jose Marin-Beloqui,Guanran Zhang,Junjun Guo,Jordan Shaikh,Thibaut Wohrer,Seyed Mehrdad Hosseini,Bowen Sun,James D. Shipp,Alexander J. Auty,Dimitri Chekulaev,Jun Ye,Yi-Chun Chin,Michael B. Sullivan,Attila J. Mozer,Ji-Seon Kim,Safa Shoaee,Tracey M. Clarke
出处
期刊:Journal of Physical Chemistry C [American Chemical Society]
标识
DOI:10.1021/acs.jpcc.1c10378
摘要

The bimolecular recombination characteristics of conjugated polymer poly[(4,4'-bis(2-ethylhexyl)dithieno[3,2-b:2',3'-d]silole)-2,6-diyl-alt-(2,5-bis 3-tetradecylthiophen-2-yl thiazolo 5,4-d thiazole)-2,5diyl] (PDTSiTTz) blended with the fullerene series PC60BM, ICMA, ICBA, and ICTA have been investigated using microsecond and femtosecond transient absorption spectroscopy, in conjunction with electroluminescence measurements and ambient photoemission spectroscopy. The non-Langevin polymer PDTSiTTz allows an inspection of intrinsic bimolecular recombination rates uninhibited by diffusion, while the low oscillator strengths of fullerenes allow polymer features to dominate, and we compare our results to those of the well-known polymer Si-PCPDTBT. Using μs-TAS, we have shown that the trap-limited decay dynamics of the PDTSiTTz polaron becomes progressively slower across the fullerene series, while those of Si-PCPDTBT are invariant. Electroluminescence measurements showed an unusual double peak in pristine PDTSiTTz, attributed to a low energy intragap charge transfer state, likely interchain in nature. Furthermore, while the pristine PDTSiTTz showed a broad, low-intensity density of states, the ICBA and ICTA blends presented a virtually identical DOS to Si-PCPDTBT and its blends. This has been attributed to a shift from a delocalized, interchain highest occupied molecular orbital (HOMO) in the pristine material to a dithienosilole-centered HOMO in the blends, likely a result of the bulky fullerenes increasing interchain separation. This HOMO localization had a side effect of progressively shifting the polymer HOMO to shallower energies, which was correlated with the observed decrease in bimolecular recombination rate and increased "trap" depth. However, since the density of tail states remained the same, this suggests that the traditional viewpoint of "trapping" being dominated by tail states may not encompass the full picture and that the breadth of the DOS may also have a strong influence on bimolecular recombination.
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