The Excited State and Charge Transfer of Two Nonfullerene Acceptors from First-Principles Many-Body Green’s Function Theory
Nonfullerene acceptors (NFAs) have shown an outstanding performance upon producing highly efficient and sustainable organic solar cells (OSC). Recently, a growing group of researchers denoted to modify the structures of acceptor−donor−acceptor-type NFAs to raise the power conversion efficiencies (PC...
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2022-01-01
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| Series: | Journal of Chemistry |
| Online Access: | http://dx.doi.org/10.1155/2022/4814131 |
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| author | Xinyue Bai Guokui Liu Yunzhi Li Guangli Zhou Xia Leng Qiying Xia Yaoyao Wei |
| author_facet | Xinyue Bai Guokui Liu Yunzhi Li Guangli Zhou Xia Leng Qiying Xia Yaoyao Wei |
| author_sort | Xinyue Bai |
| collection | DOAJ |
| description | Nonfullerene acceptors (NFAs) have shown an outstanding performance upon producing highly efficient and sustainable organic solar cells (OSC). Recently, a growing group of researchers denoted to modify the structures of acceptor−donor−acceptor-type NFAs to raise the power conversion efficiencies (PCEs) when they are blended with a variety of polymer donors in OSC. In 2020, the ketone on the ending groups of BTP-IC were substituted for sulfonyl; the new NFA named BTP-IS was synthetized. The PCE of BTP-IS based OSC is 5.25% higher than that of the BTP-IC device. Based on this, the many-body Green’s function theory, combined with other quantum chemical methods, is conducted to study their ground electronic structures, excited states, and absorption spectra. The ground-state geometries, ionization energies, and the excited state energies are deeply sensitive to exchange-correlation functionals used in calculations. The lowest excited state energies calculated by full-BSE method using DFT-PBE as the starting point is 0.07~0.14 eV smaller than that by TDDFT-PBE method, which is more consistent with experimental data. This provided a methodology for future research on similar NFA systems. The first charge-transfer states and transfer mechanism of two molecules are proposed in this paper. Furthermore, we found that the reason for more efficient charge transport in BTP-IS-based OSC is the larger ionization energies and much weaker electron-hole interaction in BTP-IS. This finding is conducive to the better application of BTP-IS in OSC field. |
| format | Article |
| id | doaj-art-5df93fc1dcda41e89f3389aa74b96c29 |
| institution | Kabale University |
| issn | 2090-9071 |
| language | English |
| publishDate | 2022-01-01 |
| publisher | Wiley |
| record_format | Article |
| series | Journal of Chemistry |
| spelling | doaj-art-5df93fc1dcda41e89f3389aa74b96c292025-08-20T03:34:45ZengWileyJournal of Chemistry2090-90712022-01-01202210.1155/2022/4814131The Excited State and Charge Transfer of Two Nonfullerene Acceptors from First-Principles Many-Body Green’s Function TheoryXinyue Bai0Guokui Liu1Yunzhi Li2Guangli Zhou3Xia Leng4Qiying Xia5Yaoyao Wei6School of Chemistry and Chemical EngineeringSchool of Chemistry and Chemical EngineeringSchool of Chemistry and Chemical EngineeringSchool of Chemistry and Chemical EngineeringSchool of Chemistry and Chemical EngineeringSchool of Chemistry and Chemical EngineeringSchool of Chemistry and Chemical EngineeringNonfullerene acceptors (NFAs) have shown an outstanding performance upon producing highly efficient and sustainable organic solar cells (OSC). Recently, a growing group of researchers denoted to modify the structures of acceptor−donor−acceptor-type NFAs to raise the power conversion efficiencies (PCEs) when they are blended with a variety of polymer donors in OSC. In 2020, the ketone on the ending groups of BTP-IC were substituted for sulfonyl; the new NFA named BTP-IS was synthetized. The PCE of BTP-IS based OSC is 5.25% higher than that of the BTP-IC device. Based on this, the many-body Green’s function theory, combined with other quantum chemical methods, is conducted to study their ground electronic structures, excited states, and absorption spectra. The ground-state geometries, ionization energies, and the excited state energies are deeply sensitive to exchange-correlation functionals used in calculations. The lowest excited state energies calculated by full-BSE method using DFT-PBE as the starting point is 0.07~0.14 eV smaller than that by TDDFT-PBE method, which is more consistent with experimental data. This provided a methodology for future research on similar NFA systems. The first charge-transfer states and transfer mechanism of two molecules are proposed in this paper. Furthermore, we found that the reason for more efficient charge transport in BTP-IS-based OSC is the larger ionization energies and much weaker electron-hole interaction in BTP-IS. This finding is conducive to the better application of BTP-IS in OSC field.http://dx.doi.org/10.1155/2022/4814131 |
| spellingShingle | Xinyue Bai Guokui Liu Yunzhi Li Guangli Zhou Xia Leng Qiying Xia Yaoyao Wei The Excited State and Charge Transfer of Two Nonfullerene Acceptors from First-Principles Many-Body Green’s Function Theory Journal of Chemistry |
| title | The Excited State and Charge Transfer of Two Nonfullerene Acceptors from First-Principles Many-Body Green’s Function Theory |
| title_full | The Excited State and Charge Transfer of Two Nonfullerene Acceptors from First-Principles Many-Body Green’s Function Theory |
| title_fullStr | The Excited State and Charge Transfer of Two Nonfullerene Acceptors from First-Principles Many-Body Green’s Function Theory |
| title_full_unstemmed | The Excited State and Charge Transfer of Two Nonfullerene Acceptors from First-Principles Many-Body Green’s Function Theory |
| title_short | The Excited State and Charge Transfer of Two Nonfullerene Acceptors from First-Principles Many-Body Green’s Function Theory |
| title_sort | excited state and charge transfer of two nonfullerene acceptors from first principles many body green s function theory |
| url | http://dx.doi.org/10.1155/2022/4814131 |
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