Separation of Intra- and Inter-Molecular Charge Carrier Mobilities of Poly(3-hexylthiophene) in Insulating Polystyrene Matrix

Fukumatsu, Takahiro; Saeki, Akinori; Seki, Shu

doi:10.2494/photopolymer.25.665

Cited by 5 publications

(5 citation statements)

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“…Therefore, the observed gigahertz local mobility (∑μ) is presumably attributed to the intramolecular hole mobility of P3HT. In fact, we have reported the separation of intra- and intermolecular mobilities by mixing an insulating polymer matrix such as poly(styrene) with P3HT and fluorene-thiophene copolymers . The intramolecular mobility of regioregular P3HT was found to be 0.12 to 0.6 cm 2 ·V –1 ·s –1 , depending on the casting solvent and thermal annealing, while that of regiorandom P3HT was two orders of magnitude smaller (0.007 cm 2 ·V –1 ·s –1 ). , The observed initial saturation in the ϕ∑μ max of P3HT, regardless of the continuous narrowing of intermolecular distance dictated by HP-XRD (Figure ), also corroborates the fact that the GHz local mobility is due to the intramolecular hole mobility rather than the intermolecular one.…”

Section: Resultsmentioning

confidence: 99%

Section: ■ Experimental Sectionmentioning

confidence: 99%

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Pressure Modulation of Backbone Conformation and Intermolecular Distance of Conjugated Polymers Toward Understanding the Dynamism of π-Figuration of their Conjugated System

et al. 2015

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Continuous tuning of the backbone conformation and interchain distance of a π-conjugated polymer is an essential prerequisite to unveil the inherent electrical and optical features of organic electronics. To this end, applying pressure in a hydrostatic medium or diamond anvil cell is a facile approach without the need for side-chain synthetic engineering. We report the development of high-pressure, time-resolved microwave conductivity (HP-TRMC) and evaluation of transient photoconductivity in the regioregular poly(3-hexylthiophene) (P3HT) film and its bulk heterojunction blend with methanofullerene (PCBM). X-ray diffraction experiments under high pressure were performed to detail the pressure dependence of π-stacking and interlamellar distances in P3HT crystallites and PCBM aggregates. The HP-TRMC results were further correlated with high-pressure Raman spectroscopy and density functional theory calculation. The increased HP-TRMC conductivity of P3HT under pressure was found to be relevant to the planarity of the backbone conformation and intramolecular hole mobility. The effects of pressure on the backbone planarity are estimated to be ∼0.3 kJ mol(-1) based on the compressibility derived from the X-ray diffraction under high pressure, suggesting the high enough energy to cause modulation of the planarity in terms of the Landau-de Gennes free energy of isolated P3HT chains as 0.23 kJ mol(-1). In contrast, the P3HT:PCBM blend showed a simple decrease in photoconductivity irrespective of the identical compressive behavior of P3HT. A mechanistic insight into the interplay of intra- and intermolecular mobilities is a key to tailoring the dynamic π-figuration associated with electrical properties, which may lead to the use of HP-TRMC for exploring divergent π-conjugated materials at the desired molecular arrangement and conformation.

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Section: Resultsmentioning

confidence: 99%

Section: ■ Experimental Sectionmentioning

confidence: 99%

Pressure Modulation of Backbone Conformation and Intermolecular Distance of Conjugated Polymers Toward Understanding the Dynamism of π-Figuration of their Conjugated System

et al. 2015

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“…However, it is generally difficult to measure the conductivity of a single molecule or a polymer chain by conventional device characterization, with the exception of nano-gap electrodes or a break-junction technique with a scanning tunnelling microscope (STM). Using the FP-TRMC method, our group has measured the intra-chain charge carrier mobility of conjugated polymers dispersed in an insulating matrix 172 and novel polymers encapsulated by cyclic side chains 116 or permethylated α-cyclodextrin. 119,122 Meanwhile, Matsuda et al proposed a unique approach to evaluate intra-molecular conductance with ESR.…”

Section: Evaluation Of Intramolecular Conductance By Esrmentioning

confidence: 99%

Charge carrier mobility in organic molecular materials probed by electromagnetic waves

Seki

Saeki

Sakurai

et al. 2014

Phys. Chem. Chem. Phys.

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129

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Charge carrier mobility is an essential parameter providing control over the performance of semiconductor devices fabricated using a variety of organic molecular materials. Recent design strategies toward molecular materials have been directed at the substitution of amorphous silicon-based semiconductors; accordingly, numerous measurement techniques have been designed and developed to probe the electronic conducting nature of organic materials bearing extremely wide structural variations in comparison with inorganic and/or metal-oxide semiconductor materials. The present perspective highlights the evaluation methodologies of charge carrier mobility in organic materials, as well as the merits and demerits of techniques examining the feasibility of organic molecules, crystals, and supramolecular assemblies in semiconductor applications. Beyond the simple substitution of amorphous silicon, we have attempted to address in this perspective the systematic use of measurement techniques for future development of organic molecular semiconductors.

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“…23) This is also evident from the amorphous nature observed in X-ray diffraction (XRD) spectrum 24) and moderate field-effect transistor (FET) hole mobility (1.1 × 10 -3 cm 2 V -1 s -1 ). 23) In addition, these results implies the overall TRMC signals are originated from the hole mobility of P3HT 33) rather than electron mobility in PFTIDG. The impact of thermal annealing was similar to the 500 nm excitation, reinforcing our presumption on the primary annealing effect on the long-lived charge carriers.…”

Section: Resultsmentioning

confidence: 88%

Ambipolar Low-bandgap Copolymers Consisting of Dithienoketopyrrole for All-Polymer Solar Cells

Ide

Koizumi

Saeki

et al. 2013

J. Photopol. Sci. Technol.

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The new low-band gap copolymers containing electron-accepting thienoisoindigo (TIDG) exhibit the low-lying lowest unoccupied molecular orbital (LUMO) at-3.8 eV. This envisions their use as n-type polymer in combination with typical p-type regioregular poly(3-hexylthiophene) (P3HT) towards all-polymer organic photovoltaics (OPV). The alternating fluorene and TIDG copolymer, PFTIDG, shows the electronic absorption maximum at 744 nm in the film states, of which spectrum is complementary to that of P3HT and thus advantageous for covering the wide solar spectrum. The laser and Xe-flash time-resolved microwave conductivity (TRMC) evaluations were performed for screening the effects of p/n blend ratio and thermal annealing in bulk heterojunction framework. The power conversion efficiency of 0.06% was obtained for pre-annealed P3HT:PFTIDG = 1:1 together with a high open circuit voltage of 0.92 V, which is suggestive of ambipolar characteristics of PFTIDG.

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Separation of Intra- and Inter-Molecular Charge Carrier Mobilities of Poly(3-hexylthiophene) in Insulating Polystyrene Matrix

Cited by 5 publications

References 16 publications

Pressure Modulation of Backbone Conformation and Intermolecular Distance of Conjugated Polymers Toward Understanding the Dynamism of π-Figuration of their Conjugated System

Pressure Modulation of Backbone Conformation and Intermolecular Distance of Conjugated Polymers Toward Understanding the Dynamism of π-Figuration of their Conjugated System

Charge carrier mobility in organic molecular materials probed by electromagnetic waves

Ambipolar Low-bandgap Copolymers Consisting of Dithienoketopyrrole for All-Polymer Solar Cells

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