2D coherent charge transport in highly ordered conducting polymers doped by solid state diffusion

Kang, Keehoon; Watanabe, Shun; Broch, Katharina; Sepe, Alessandro; Brown, Adam R.; Nasrallah, Iyad; Nikolka, Mark; Fei, Zhuping; Heeney, Martin; Matsumoto, Daisuke; Marumoto, Kazuhiro; Tanaka, Hisaaki; Kuroda, Shin Ichi; Sirringhaus, Henning

doi:10.1038/nmat4634

Cited by 404 publications

(516 citation statements)

References 48 publications

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“…Particularly, film thickness should be considered in the analysis of transport in insulator-wrapped s-SWNT films. Our results could be used in materials design strategies including surfactant removal [35,36], dopant miscibility [37], and thin film integration [38]. …”

Section: Resultsmentioning

confidence: 99%

Thickness-dependent thermoelectric power factor of polymer-functionalized semiconducting carbon nanotube thin films

Nonoguchi

Takata

Goto

et al. 2018

Science and Technology of Advanced Materials

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The effects of polymer structures on the thermoelectric properties of polymer-wrapped semiconducting carbon nanotubes have yet to be clarified for elucidating intrinsic transport properties. We systematically investigate thickness dependence of thermoelectric transport in thin films containing networks of conjugated polymer-wrapped semiconducting carbon nanotubes. Well-controlled doping experiments suggest that the doping homogeneity and then in-plane electrical conductivity significantly depend on film thickness and polymer species. This understanding leads to achieving thermoelectric power factors as high as 412 μW m−1 K−2 in thin carbon nanotube films. This work presents a standard platform for investigating the thermoelectric properties of nanotubes.

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Section: Resultsmentioning

confidence: 99%

Thickness-dependent thermoelectric power factor of polymer-functionalized semiconducting carbon nanotube thin films

Nonoguchi

Takata

Goto

et al. 2018

Science and Technology of Advanced Materials

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“…The results indicate that 2D coherent transport can be realized even in commonplace polymer films fabricated by simple drop-casting using a popular material, rather than only in highly crystalline materials. [37,38] Our findings could provide not only new insight into the conductance anisotropy in PEDOT:PSS, but also the ability to explore a wealth of 2D quantum physics phenomena hidden in polymers. …”

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confidence: 90%

Mesoscopic 2D Charge Transport in Commonplace PEDOT:PSS Films

Honma

Itoh

Masunaga

et al. 2018

Adv Elect Materials

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The correlation between the transport properties and structural degrees of freedom of conducting polymers is a central concern in both practical applications and scientific research. In this study, we demonstrated the existence of mesoscopic two-dimensional (2D) coherent charge transport in poly(3,4-ethylenedioxythiophene):poly-(styrenesulfonate) (PEDOT:PSS) film by performing structural investigations and high-field magnetoconductance (MC) measurements in magnetic fields of up to 15 T. We succeeded in observing marked positive MCs reflecting 2D electronic states in a conventional drop-cast film. This low-dimensional feature is surprising, since PEDOT:PSS-a mixture of two different polymers-seems to be significantly different from crystalline 2D materials in the viewpoint of the structural inhomogeneity, especially in popular drop-cast thick films. The results of the structural experiments suggest that such 2D transport originates from the nanometer-scale self-assembled laminated structure, which is composed of PEDOT nanocrystals wrapped by insulating sheets consisting of amorphous PSSs. These results indicate that charge transport in the PEDOT:PSS film can be divided into two regimes: mesoscopic 2D coherent tunneling and macroscopic three-dimensional hopping among 2D states. Our findings elucidate the hieratical nature of charge transport in the PEDOT:PSS film, which could provide new insight into a recent engineering concern, i.e., the reduction of the out-of-plane conductance.Conductive polymers are becoming indispensable in both scientific research and practical applications because of their advantageous features, such as mechanical flexibility, low toxicity, and the potential for use in low-cost device fabrication via printing processes. In particular, poly(3,4-ethylenedioxythiophene):poly(styrenesulfonate) (PEDOT:PSS, which is produced by doping PEDOT with PSS) is one of the most commonly used polymers owing to its beneficial electric and thermoelectric properties, good stability under ambient conditions, and visible-light transmittance in thin-film form.[1-8] Electrical conductivities exceeding 1000 S/cm have routinely been achieved through the development of efficient methods, in particular, the addition of polar solvents to aqueous PEDOT:PSS solutions; [9][10][11] however, the charge transport mechanism is still not well understood in spite of its widespread utilization. The electrical properties of PEDOT:PSS films are strongly related to their complicated macromolecular structures; hence, clarifying the correlations between their electrical and structural properties is an active area of investigation in polymer science.The anisotropic conductance, namely, the reduction of outof-plane conductivity, in highly conductive PEDOT:PSS films is one of the crucial issues that must be unraveled for future applications. [12][13][14][15][16][17] Previous studies have indicated that the out-of-plane conductivity tends to be significantly less than the in-plane conductivity. Nardes et al. [12] reported an anisotropy...

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“…Although the production of high-performance polymers has been demonstrated, overoxidation leads to severe structural distortions. [39,40] Here we develop a new process that achieves superior metallic properties but overcomes the prior reliance on lattice-disrupting metal dopants. The o-CVD is performed at ambient pressure and uses nitrogen as carrier gas, which is saturated with the monomer ethylene-(3,4-dioxythiophene) (EDOT).…”

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confidence: 99%

Anderson‐Localization and the Mott–Ioffe–Regel Limit in Glassy‐Metallic PEDOT

Farka

Coskun

Gąsiorowski

et al. 2017

Adv Elect Materials

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There exists a tremendous interest in metallic polymers as they combine facile processing, high conductivity and transparency. However, to date no straightforward method has been found to engineer a system that unites high doping and high order. [1][2][3][4][5][6] The apparent conflict lies in the nature of doping of a conducting polymer, which occurs through a distinct mechanism compared to inorganic semiconductors. Severe lattice distortions arise in the doping of conducting polymers as a result of the penetration of ions into the system. Consequently, the solid-state order becomes disrupted-it transforms from a former homogeneous organic vander-Waals crystal into a disordered salt. To form a substantial degree of order, growth methods have to consider the effect of ion penetration. [7][8][9][10][11][12][13][14][15][16] Small molecular systems have the advantage that they can be dissolved in polar solvents. Thus they can be grown in the doped form as a salt dissolved from Conductive polymers represent a rare case in which free-carrier absorption is shifted to the far-infrared-an attractive advantage in light of the requirement of highly transparent conductors across the visible and near-infrared. Unfortunately, prior approaches to doping these polymers-imperative for high conductance-have consistently led to strong localization arising from fluctuating band alignment among polymer chains. Here, this study overcomes this problem of doping-induced Anderson localization for the first time in polymers by developing a new conductive polymer synthesis strategy. This study achieves polymerization and doping simultaneously, thereby using an alternative nonmetal oxidant and thereby avoiding the introduction of excess energy that normally arises from exergonic polymerization. The resulting conductive polymer is the first to provide electron coherence in a metallic polymer thin film. The conductivity reaches a remarkable 3300 S cm −1 at 1.8 K and the mean electron scattering length a record 330 Å. This enhancement drives the glassy metal transition in the vicinity of the Mott-Ioffe-Regel (MIR) limit. The new metallic polymer achieves 10 −2 Ω −1 figure of merit, making it a contender for transparent conductive contacts previously only accessible using inorganics. The new material offers a uniquely broad transparency window spanning the UV to the mid-infrared. The ORCID identification number(s) for the author(s) of this article can be found under http://dx

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2D coherent charge transport in highly ordered conducting polymers doped by solid state diffusion

Cited by 404 publications

References 48 publications

Thickness-dependent thermoelectric power factor of polymer-functionalized semiconducting carbon nanotube thin films

Thickness-dependent thermoelectric power factor of polymer-functionalized semiconducting carbon nanotube thin films

Mesoscopic 2D Charge Transport in Commonplace PEDOT:PSS Films

Anderson‐Localization and the Mott–Ioffe–Regel Limit in Glassy‐Metallic PEDOT

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