Intra-molecular Charge Transfer and Electron Delocalization in Non-fullerene Organic Solar Cells

Wu, Qinghe; Zhao, Donglin; Goldey, Matthew B.; Filatov, Alexander S.; Sharapov, Valerii; Colon, Yamil J.; Cai, Zhengxu; Chen, Wei; de Pablo, Juan; Galli, Giulia; Yu, Luping

doi:10.1021/acsami.7b18717

Title: Intra-molecular Charge Transfer and Electron Delocalization in Non-fullerene Organic Solar Cells

Journal Article · Fri Mar 02 00:00:00 EST 2018 · ACS Applied Materials and Interfaces

DOI:https://doi.org/10.1021/acsami.7b18717· OSTI ID:1433912

^[1]; Zhao, Donglin ^[2];

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^[2]; Colon, Yamil J. ^[4];

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^[4]; Galli, Giulia ^[4]; Yu, Luping ^[2]

Shantou Univ., Guangdong (China). Dept. of Chemistry, Key Lab. for Preparation and Application of Ordered Structural Materials of Guangdong Province
Univ. of Chicago, IL (United States). Dept. of Chemistry, The James Franck Inst.
Univ. of Chicago, IL (United States). Inst. for Molecular Engineering
Argonne National Lab. (ANL), Argonne, IL (United States). Materials Science Division, Inst. for Molecular Engineering; Univ. of Chicago, IL (United States). Inst. for Molecular Engineering

Two types of electron acceptors were synthesized by coupling two kinds of electron-rich cores with four equivalent perylene diimides (PDIs) at the a position. With fully aromatic cores, TPB and TPSe have pi-orbitals spread continuously over the whole aromatic conjugated backbone, unlike TPC and TPSi, which contain isolated PDI units due to the use of a tetrahedron carbon or silicon linker. Density functional theory calculations of the projected density of states showed that the highest occupied molecular orbital (HOMO) and lowest unoccupied molecular orbital (LUMO) for TPB are localized in separate regions of space. Further, the LUMO of TPB shows a greater contribution from the orbitals belonging to the connective core of the molecules than that of TPC. Overall, the properties of the HOMO and LUMO point at increased intra-molecular delocalization of negative charge carriers for TPB and TPSe than for TPC and TPSi and hence at a more facile intra-molecular charge transfer for the former. The film absorption and emission spectra showed evidences for the inter -molecular electron delocalization in TPB and TPSe, which is consistent with the network structure revealed by X-ray diffraction studies on single crystals of TPB. These features benefit the formation of charge transfer states and/or facilitate charge transport. Thus, higher electron mobility and higher charge dissociation probabilities under J_sc condition were observed in blend films of TPB:PTB7-Th and TPSe:PTB7-Th than those in TPC:PTB7Th and TPSi:PTB7-Th blend films. As a result, the J_sc and fill factor values of 15.02 mA/cm², 0.58 and 14.36 mA/cm², 0.55 for TPB- and TPSe-based solar cell are observed, whereas those for TPC and TPSi are 11.55 mA/cm², 0.47 and 10.35 mA/cm², 0.42, respectively.

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Research Organization:: Argonne National Laboratory (ANL), Argonne, IL (United States); Energy Frontier Research Centers (EFRC) (United States). Argonne-Northwestern Solar Energy Research Center (ANSER)

Sponsoring Organization:: USDOE Office of Science (SC), Basic Energy Sciences (BES); National Science Foundation (NSF)

Grant/Contract Number:: AC02-06CH11357; SC0001059; DMR-1263006; CHE-1346572

OSTI ID:: 1433912

Journal Information:: ACS Applied Materials and Interfaces, Vol. 10, Issue 12; ISSN 1944-8244

Publisher:: American Chemical Society (ACS)Copyright Statement

Country of Publication:: United States

Language:: English

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Cited by: 19 works

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25 ENERGY STORAGE
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electron delocalization
intra-molecular charge transfer
non-fullerene electron acceptor
organic solar cell
perylene diimide