Enhanced Carrier Mobility and Thermoelectric Performance by Nanostructure Engineering of PEDOT Thin Films Fabricated via the OCVD Method Using SbCl5 Oxidant

IF 18.5 1区 材料科学 Q1 CHEMISTRY, MULTIDISCIPLINARY
Meysam Heydari Gharahcheshmeh, Brian Dautel, Kafil Chowdhury
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Abstract

Air-stable, lightweight, and electrically conductive conjugated polymers have attracted significant attention for thermoelectric applications, especially in low-temperature environments. However, their low carrier mobility has limited broader adoption. This study addresses this challenge by investigating the nanostructure of poly(3,4-ethylenedioxythiophene) (PEDOT) thin films fabricated via oxidative chemical vapor deposition (oCVD) at various deposition temperatures. Through systematic control of the semi-crystalline orientation and π–π stacking distance, a substantial enhancement in carrier mobility (23.58 ± 1.71 cm2 V−1 s−1) and electrical conductivity (6345 ± 210 S cm−1) is achieved. The thermoelectric power factor demonstrates a direct correlation with deposition temperature, achieving a maximum value of 112.57 ± 4.33 µW m−1 K−2. PEDOT thin films fabricated at higher deposition temperatures show minimal reductions in electrical conductivity as absolute temperature decreased, reflecting a lower resistivity ratio and extended metallic state, as indicated by the metal–insulator transition in the Zabrodskii plot. Incorporating the Seebeck coefficient into the parabolic energy band diagram revealed strong agreement between theoretical and experimental carrier mobility, while also indicating that the energy barrier for intercrystalline charge transport decreases as deposition temperature increases. The highly face-on orientation and reduced π–π stacking distance in PEDOT thin films facilitate quasi-1D conduction, thereby enhancing carrier mobility.

Abstract Image

用SbCl5氧化剂OCVD法制备PEDOT薄膜的纳米结构工程提高载流子迁移率和热电性能
空气稳定、重量轻、导电的共轭聚合物在热电应用中引起了极大的关注,特别是在低温环境中。然而,它们的低载波移动性限制了更广泛的采用。本研究通过研究在不同沉积温度下通过氧化化学气相沉积(oCVD)制备的聚(3,4‐乙烯二氧噻吩)(PEDOT)薄膜的纳米结构来解决这一挑战。通过系统控制半晶取向和π -π堆积距离,载流子迁移率(23.58±1.71 cm2 V−1 s−1)和导电性(6345±210 s cm−1)得到了显著提高。热电功率因数与沉积温度直接相关,最大值为112.57±4.33µW m−1 K−2。随着绝对温度的降低,在较高沉积温度下制备的PEDOT薄膜的电导率下降最小,反映了更低的电阻率和延长的金属状态,正如Zabrodskii图中的金属-绝缘体转变所示。将塞贝克系数纳入抛物能带图,揭示了理论和实验载流子迁移率之间的强烈一致性,同时也表明晶间电荷输运的能量势垒随着沉积温度的升高而降低。PEDOT薄膜中高度的面朝取向和减小的π -π堆积距离有利于准一维导电,从而提高载流子迁移率。
本文章由计算机程序翻译,如有差异,请以英文原文为准。
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来源期刊
Advanced Functional Materials
Advanced Functional Materials 工程技术-材料科学:综合
CiteScore
29.50
自引率
4.20%
发文量
2086
审稿时长
2.1 months
期刊介绍: Firmly established as a top-tier materials science journal, Advanced Functional Materials reports breakthrough research in all aspects of materials science, including nanotechnology, chemistry, physics, and biology every week. Advanced Functional Materials is known for its rapid and fair peer review, quality content, and high impact, making it the first choice of the international materials science community.
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