Achieving ideal transistor characteristics in conjugated polymer semiconductors

Mingfei Xiao¹, Xinglong Ren¹, Kangyu Ji¹, Sein Chung², Xiaoyu Shi³, Jie Han³, Zefan Yao⁴, Xudong Tao⁵, Szymon J Zelewski^{1

6}, Mark Nikolka¹, Youcheng Zhang¹, Zhilong Zhang¹, Zichen Wang¹, Nathan Jay⁵, Ian Jacobs¹, Weijing Wu⁷, Han Yu⁸, Yarjan Abdul Samad⁹, Samuel D Stranks¹, Boseok Kang¹⁰, Kilwon Cho², Jin Xie³, He Yan⁸, Shangshang Chen³, Henning Sirringhaus¹

Affiliations

¹ Cavendish Laboratory, University of Cambridge, J.J. Thomson Ave., Cambridge CB3 0HE, UK.
² Department of Chemical Engineering, Pohang University of Science and Technology Pohang, Pohang 790-784, South Korea.
³ State Key Laboratory of Coordination Chemistry, School of Chemistry and Chemical Engineering, Nanjing University, Nanjing 210023, P. R. of China.
⁴ College of Chemistry and Molecular Engineering, Peking University, Beijing 100871, P. R. of China.
⁵ Electrical Engineering Division, Department of Engineering, University of Cambridge, 9 JJ Thomson Ave., Cambridge CB3 0FA, UK.
⁶ Department of Semiconductor Materials Engineering, Faculty of Fundamental Problems of Technology, Wrocław University of Science and Technology, Wybrzeże Wyspiańskiego 27, 50-370 Wrocław, Poland.
⁷ Institute of Polymer Optoelectronic Materials and Devices, State Key Laboratory of Luminescent Materials and Devices, South China University of Technology, Guangzhou 510640, P. R. of China.
⁸ Department of Chemistry, Guangdong-Hong Kong-Macao Joint Laboratory of Optoelectronic and Magnetic Functional Materials, Energy Institute and Hong Kong Branch of Chinese National Engineering Research Center for Tissue Restoration & Reconstruction, Hong Kong University of Science and Technology, Clear Water Bay, Kowloon, Hong Kong 999077, P. R. of China.
⁹ Department of Aerospace Engineering, Khalifa University, Abu Dhabi 127788, UAE.
¹⁰ SKKU Advanced Institute of Nanotechnology and Department of Nano Engineering, Sungkyunkwan University, Suwon 16419, Republic of Korea.

PMID: 37267357
PMCID: PMC10413658
DOI: 10.1126/sciadv.adg8659

Achieving ideal transistor characteristics in conjugated polymer semiconductors

Mingfei Xiao et al. Sci Adv. 2023.

. 2023 Jun 2;9(22):eadg8659.

doi: 10.1126/sciadv.adg8659. Epub 2023 Jun 2.

Authors

Affiliations

¹ Cavendish Laboratory, University of Cambridge, J.J. Thomson Ave., Cambridge CB3 0HE, UK.
² Department of Chemical Engineering, Pohang University of Science and Technology Pohang, Pohang 790-784, South Korea.
³ State Key Laboratory of Coordination Chemistry, School of Chemistry and Chemical Engineering, Nanjing University, Nanjing 210023, P. R. of China.
⁴ College of Chemistry and Molecular Engineering, Peking University, Beijing 100871, P. R. of China.
⁵ Electrical Engineering Division, Department of Engineering, University of Cambridge, 9 JJ Thomson Ave., Cambridge CB3 0FA, UK.
⁶ Department of Semiconductor Materials Engineering, Faculty of Fundamental Problems of Technology, Wrocław University of Science and Technology, Wybrzeże Wyspiańskiego 27, 50-370 Wrocław, Poland.
⁷ Institute of Polymer Optoelectronic Materials and Devices, State Key Laboratory of Luminescent Materials and Devices, South China University of Technology, Guangzhou 510640, P. R. of China.
⁸ Department of Chemistry, Guangdong-Hong Kong-Macao Joint Laboratory of Optoelectronic and Magnetic Functional Materials, Energy Institute and Hong Kong Branch of Chinese National Engineering Research Center for Tissue Restoration & Reconstruction, Hong Kong University of Science and Technology, Clear Water Bay, Kowloon, Hong Kong 999077, P. R. of China.
⁹ Department of Aerospace Engineering, Khalifa University, Abu Dhabi 127788, UAE.
¹⁰ SKKU Advanced Institute of Nanotechnology and Department of Nano Engineering, Sungkyunkwan University, Suwon 16419, Republic of Korea.

PMID: 37267357
PMCID: PMC10413658
DOI: 10.1126/sciadv.adg8659

Abstract

Organic thin-film transistors (OTFTs) with ideal behavior are highly desired, because nonideal devices may overestimate the intrinsic property and yield inferior performance in applications. In reality, most polymer OTFTs reported in the literature do not exhibit ideal characteristics. Supported by a structure-property relationship study of several low-disorder conjugated polymers, here, we present an empirical selection rule for polymer candidates for textbook-like OTFTs with high reliability factors (100% for ideal transistors). The successful candidates should have low energetic disorder along their backbones and form thin films with spatially uniform energetic landscapes. We demonstrate that these requirements are satisfied in the semicrystalline polymer PffBT4T-2DT, which exhibits a reliability factor (~100%) that is exceptionally high for polymer devices, rendering it an ideal candidate for OTFT applications. Our findings broaden the selection of polymer semiconductors with textbook-like OTFT characteristics and would shed light upon the molecular design criteria for next-generation polymer semiconductors.

PubMed Disclaimer

Figures

**Fig. 1.. Molecular structures and energetic disorder of conjugated polymers.**
(A) Molecular structures of IDT-BT, PffBT4T-2DT, and N2200. (B) PDS spectrum of PffBT4T-2DT thin film with extracted E_U. a.u., arbitrary units. (C) ER-EIS of four different polymers (IDT-BT, N2200, PBTTT, and PffBT4T-2DT). For p-type IDT-BT, PBTTT, and PffBT4T-2DT, their highest occupied molecular orbital bands are probed; for n-type N2200, its lowest unoccupied molecular orbital band is probed. The characteristic band tail broadening energy is defined as the inverse of the slope. (D) Distribution of local PL COM compared with bulk PL COM of four different polymers.

**Fig. 2.. Analysis of GIWAXS and carbon K-edge NEXAFS spectra of PffBT4T-2DT films.**
(A) 2D GIWAXS patterns of spin-coated PffBT4T-2DT films (α_c = critical angle of the thin film, α_i = incidence angle of the x-ray beam). (B) Corresponding GIWAXS line profile along the in-plane/out-of-plane directions. (C) Population ratio analysis of edge-on, face-on, and isotropic crystals. (D) Total electron yield (TEY) mode NEXAFS spectra with four incidence angles (θ) for the top surface of PffBT4T-2DT films (left) and the π* NEXAFS spectra intensity as a function of cos²(θ) with linear fitting (right).

**Fig. 3.. Performance of OTFTs based on PffBT4T-2DT.**
(A and D) Linear and saturation transfer curves measured on a representative top-gate, bottom-contact OTFT (L = 20 μm, W = 1 mm) fabricated from spin-coated, as cast PffBT4T-2DT films. (B and E) Linear and saturation mobility calculated from the transfer curves measured on the same device. (C and F) Output curves measured on the same device. (D) to (F) Transfer curves, mobility, and output curves measured after 50 days of air exposure. (G) Reliability factor of the device shown in (D): The red line is the linear fit of the transfer curve, and the blue line represents an ideal transistor showing the same maximum current but following the standard transistor equations. (H) Temperature-dependent saturation mobility calculated from the transfer curves measured on the same device. (I) Activation energy of device extracted from the temperature-dependent saturation mobility at V_G = −60 V.

**Fig. 4.. Seebeck measurements of OTFTs based on PffBT4T-2DT.**
(A) Seebeck coefficients versus the logarithm of carrier concentration for PffBT4T-2DT OTFT at 295 K. (B) Temperature-dependent Seebeck coefficient versus the logarithm of carrier concentration for PffBT4T-2DT OTFT.

See this image and copyright information in PMC

References

1. M. Zhu, Y. Guo, Y. Liu, A thriving decade: rational design, green synthesis, and cutting-edge applications of isoindigo-based conjugated polymers in organic field-effect transistors. Sci. China Chem. 65, 1225–1264 (2022).
1. S. Wang, S. Fabiano, S. Himmelberger, S. Puzinas, X. Crispin, A. Salleo, M. Berggren, Experimental evidence that short-range intermolecular aggregation is sufficient for efficient charge transport in conjugated polymers. Proc. Natl. Acad. Sci. U.S.A. 112, 10599–10604 (2015). - PMC - PubMed
1. Y. Zhao, C. Su, G. Shen, Z. Xie, W. Xiao, Y. Fu, S. Inal, Q. Wang, Y. Wang, W. Yue, I. McCulloch, D. He, Donor Engineering Tuning the Analog Switching Range and Operational Stability of Organic Synaptic Transistors for Neuromorphic Systems. Adv. Funct. Mater. 32, 2205744 (2022).
1. S. Chen, S. Zhu, Z. Lin, J. Peng, Transforming Polymorphs via Meniscus-Assisted Solution-Shearing Conjugated Polymers for Organic Field-Effect Transistors. ACS Nano 16, 11194–11203 (2022). - PubMed
1. C. S. Buga, J. C. Viana, A Review on Materials and Technologies for Organic Large-Area Electronics. Adv. Mater. Technol. 6, 2001016 (2021).

LinkOut - more resources

Full Text Sources

Save citation to file

Email citation

Add to Collections

Add to My Bibliography

Your saved search

Create a file for external citation management software

Your RSS Feed

Achieving ideal transistor characteristics in conjugated polymer semiconductors

Affiliations

Achieving ideal transistor characteristics in conjugated polymer semiconductors

Authors

Affiliations

Abstract

Figures

References

LinkOut - more resources

Full Text Sources