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High-mobility semiconducting polymers with different spin ground states

Xiao-Xiang Chen1,2*, Jia-Tong Li1*, Yu-Hui Fang2*, Xin-Yu Deng1*, Xue-Qing Wang1*, Guangchao Liu1*, Yunfei Wang3*, Xiaodan Gu3*, Shang-Da Jiang4*, Ting Lei1,5*

1 Key Laboratory of Polymer Chemistry and Physics of Ministry of Education, School of Materials Science and Engineering, Peking University, Beijing 100871, China.

2 College of Chemistry and Molecular Engineering, Peking University, Beijing 100871, China.

3 School of Polymer Science and Engineering, Center for Optoelectronic Materials and Devices, The University of Southern Mississippi, Hattiesburg, MS 39406, USA.

4 School of Chemistry and Chemical Engineering, South China University of Technology, Guangzhou, China.

5 Beijing Key Laboratory for Magnetoelectric Materials and Devices, Peking University, Beijing 100871, China.

* Corresponding authors emails: xiaoxiangchen@pku.edu.cn, guatong@pku.edu.cn, yhfang@pku.edu.cn, xinyudeng@stu.pku.edu.cn, xqwang@stu.pku.edu.cn, gcliu@pku.edu.cn, yunfei.wang@usm.edu, xiaodan.gu@usm.edu, jiangsd@scut.edu.cn, tinglei@pku.edu.cn
DOI10.24435/materialscloud:58-27 [version v1]

Publication date: Apr 01, 2022

How to cite this record

Xiao-Xiang Chen, Jia-Tong Li, Yu-Hui Fang, Xin-Yu Deng, Xue-Qing Wang, Guangchao Liu, Yunfei Wang, Xiaodan Gu, Shang-Da Jiang, Ting Lei, High-mobility semiconducting polymers with different spin ground states, Materials Cloud Archive 2022.46 (2022), doi: 10.24435/materialscloud:58-27.


Organic semiconductors with high-spin ground states are fascinating because they could enable fundamental understanding on the spin-related phenomenon in light element and provide opportunities for organic magnetic and quantum materials. Although high-spin ground states have been observed in some quinoidal type small molecules or doped organic semiconductors, semiconducting polymers with high-spin at their neutral ground state are rarely reported. Here we report three high-mobility semiconducting polymers with different spin ground states. We show that polymer building blocks with small singlet-triplet energy gap (ΔES-T) could enable small ΔES-T gap and increase the diradical character in copolymers. We demonstrate that the electronic structure, spin density, and solid-state interchain interactions in the high-spin polymers are crucial for their ground states. Polymers with a triplet ground state (S = 1) could exhibit doublet (S = 1/2) behavior due to different spin distributions and solid-state interchain spin-spin interactions. Besides, these polymers showed outstanding charge transport properties with high hole/electron mobilities and can be both n- and p-doped with superior conductivities. Our results demonstrate a rational approach to high-mobility semiconducting polymers with different spin ground states.

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File name Size Description
Fig. 3 and Fig. 4.zip
504.1 KiB Open data for Fig. 3 and Fig. 4 in the manuscript. Fig.3 : Calculated potential energy scans (PES) of the dihedral angles φ. Fig 4: Magnetic property characterization and DFT calculation
Fig. 5 and Fig. 6.zip
162.3 KiB Open data for Fig. 5 and Fig. 6 in the manuscript. Fig. 5: Magnetic characterization for two polymers. Fig. 6: Thin film morphology and device characterization.
Fig. S1-3.zip
734.5 KiB Open data for Fig. S1-3 in the SI. Fig. S1:DFT calculations for the evaluation of polymer building block planarity. Fig. S2-3: The thermal stability, cyclic voltammograms, and inductively coupled plasma (ICP) emission spectroscopy for the trace metal analysis of the polymers
Fig. S4-5.zip
433.0 KiB Open data for Fig. S4-5 in the SI. Fig. S4-5:EPR and SQUID measurement.
Fig. S6-9.zip
199.2 KiB Open data for Fig. S6-9 in the SI. Fig. S6-9: Quantitative EPR measurement for EPR spin susceptibility of p(TDPP-BBT).
Fig. S10-11.zip
694.3 KiB Open data for Fig. S10-11 in the SI. Fig. S10-11: Temperature-dependent UV-vis absorption spectra of p(TDPP-TQ) and p(TDPP-BBT).
Fig. S17-19.zip
57.6 KiB Open data for Fig. S17-19 in the Manuscript. Fig. S17-19: DFT calculations of oligomers and dimers.
Fig. S21.zip
54.0 KiB Open data for Fig. S21 in the SI. Fig. S21: Evolution of the binding energy of the cofacially stacked polymer chains with different degrees of translation of one polymer chain along the long axis.
Fig. S25-29.zip
367.3 KiB Open data for Fig. S25-29 in the SI. Fig. S25-29: OFET device characterization.
Fig. S31-34.zip
676.4 KiB Open data for Fig. S31-34 in the SI. Fig. S31-34: Polymer doping and electrical conductivity measurement and thin film characterization.


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External references

Journal reference (Preprint where the data is discussed. This paper has been accepted by Nature Communications.)


Organic semiconductor High-spin materials High-mobility polymers

Version history:

2022.46 (version v1) [This version] Apr 01, 2022 DOI10.24435/materialscloud:58-27