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Dynamics of Quasi-ordered Structure in a Regio-regulated pi-Conjugated Polymer:Poly(4-methylthiazole-2,5-diyl)

Seiichiro Mori·Yoshio Inoue·Takakazu Yamamoto·Naoki Asakawa
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Abstract

Dynamics of regio-regulated Poly(4-methylthiazole-2,5-diyl) [HH-P4MeTz] was inves tigated by solid-state 1H, 2D, 13C NMR spectroscopies, and differential scanning calorimetry(DSC) measurements. DSC, 2D quadrupolar echo NMR, 13C cross-polarization and magic-angle spinning(CPMAS) NMR, and 2D spin-echo(2DSE) CPMAS NMR spectroscopy suggest existence of a quasi-ordered phase in which backbone twists take place with weakened pi-stackings. Two-dimensional exchange 2D NMR(2DEX) detected slow dynamics with a rate of an order of 10^2Hz for the CD_3 group in d_3-HH-P4MeTz at 288K. The frequency dependence of proton longitudinal relaxation rate at 288K shows a omega^-1/2 dependence, which is due to the one-dimensional diffusion-like motion of backbone conformational modulation waves. The diffusion rate was estimated as 3+/-2 GHz, which was approximately 10^7 times larger than that estimated by 2DEX NMR measurements. These results suggest that there exists anomalous dispersion of modulation waves in HH-P4MeTz. The one-dimensional group velocity of the wave packet is responsible for the behavior of proton longitudinal relaxation time. On the other hand, the 2DEX NMR is sensitive to phase velocity of the nutation of methyl groups that is associated with backbone twists. From proton T_1 and T_2 measurements, the activation energy was estimated as 2.9 and 3.4 kcal/mol, respectively. These were in agreement with 3.0 kcal/mol determined by Moller-Plesset(MP2) molecular orbital(MO) calculation. We also performed chemical shielding calculation of the methyl-carbon in order to understand chemical shift tensor behavior, leading to the fact that a quasi-ordered phase coexist with the crystalline phase.

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Seiichiro Mori, Yoshio Inoue, Takakazu Yamamoto, Naoki Asakawa. 2004-12-16. Dynamics of Quasi-ordered Structure in a Regio-regulated pi-Conjugated Polymer:Poly(4-methylthiazole-2,5-diyl). https://doi.org/10.1103/physrevb.71.054205

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