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High n-type and p-type conductivities and power factors achieved in a single conjugated polymer.

ABSTRACT: The charge transport properties of conjugated polymers are commonly limited by the energetic disorder. Recently, several amorphous conjugated polymers with planar backbone conformations and low energetic disorder have been investigated for applications in field-effect transistors and thermoelectrics. However, there is a lack of strategy to finely tune the interchain π-π contacts of these polymers that severely restricts the energetic disorder of interchain charge transport. Here, we demonstrate that it is feasible to achieve excellent conductivity and thermoelectric performance in polymers based on thiophene-fused benzodifurandione oligo(p-phenylenevinylene) through reducing the crystallization rate of side chains and, in this way, carefully controlling the degree of interchain π-π contacts. N-type (p-type) conductivities of more than 100 S cm^-1 (400 S cm^-1) and power factors of more than 200 μW m^-1 K^-2 (100 μW m^-1 K^-2) were achieved within a single polymer doped by different dopants. It further demonstrated the state-of-the-art power output of the first flexible single-polymer thermoelectric generator.

SUBMITTER: Yu ZD

PROVIDER: S-EPMC9956111 | biostudies-literature | 2023 Feb

REPOSITORIES: biostudies-literature

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High n-type and p-type conductivities and power factors achieved in a single conjugated polymer.

Yu Zi-Di ZD Lu Yang Y Wang Zi-Yuan ZY Un Hio-Ieng HI Zelewski Szymon J SJ Cui Ying Y You Hao-Yang HY Liu Yi Y Xie Ke-Feng KF Yao Ze-Fan ZF He Yu-Cheng YC Wang Jie-Yu JY Hu Wen-Bing WB Sirringhaus Henning H Pei Jian J

Science advances 20230224 8

The charge transport properties of conjugated polymers are commonly limited by the energetic disorder. Recently, several amorphous conjugated polymers with planar backbone conformations and low energetic disorder have been investigated for applications in field-effect transistors and thermoelectrics. However, there is a lack of strategy to finely tune the interchain π-π contacts of these polymers that severely restricts the energetic disorder of interchain charge transport. Here, we demonstrate ...[more]

PMID: 36827372

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Project description:Single molecule photoluminescence (PL) spectroscopy of conjugated polymers has shed new light on the complex structure⁻function relationships of these materials. Although extensive work has been carried out using polarization and excitation intensity modulated experiments to elucidate conformation-dependent photophysics, surprisingly little attention has been given to information contained in the PL spectral line shapes. We investigate single molecule PL spectra of the prototypical conjugated polymer poly[2-methoxy-5-(2-ethylhexyloxy)-1,4-phenylenevinylene] (MEH-PPV) which exists in at least two emissive conformers and can only be observed at dilute levels. Using a model based on the well-known "Missing Mode Effect" (MIME), we show that vibronic progression intervals for MEH-PPV conformers can be explained by relative contributions from particular skeletal vibrational modes. Here, observed progression intervals do not match any ground state Raman active vibrational frequency and instead represent a coalescence of multiple modes in the frequency domain. For example, the higher energy emitting "blue" MEH-PPV form exhibits PL maxima at ~18,200 cm-1 with characteristic MIME progression intervals of ~1200⁻1350 cm-1, whereas the lower energy emitting "red" form peaks at ~17,100 cm-1 with intervals in the range of ~1350⁻1450 cm-1. The main differences in blue and red MEH-PPV chromophores lie in the intra-chain order, or, planarity of monomers within a chromophore segment. We demonstrate that the Raman-active out-of-plane C⁻H wag of the MEH-PPV vinylene group (~966 cm-1) has the greatest influence in determining the observed vibronic progression MIME interval. Namely, larger displacements (intensities)-indicating lower intra-chain order-lower the effective MIME interval. This simple model provides useful insights into the conformational characteristics of the heterogeneous chromophore landscape without requiring costly and time-consuming low temperature or single molecule Raman capabilities.

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High n-type and p-type conductivities and power factors achieved in a single conjugated polymer.

Publications

High n-type and p-type conductivities and power factors achieved in a single conjugated polymer.

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