期刊
MACROMOLECULES
卷 49, 期 24, 页码 9553-9560出版社
AMER CHEMICAL SOC
DOI: 10.1021/acs.macromol.6b02077
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资金
- German Research Foundation DFG [HI1508/2, GRK1640]
- Bavarian State Ministry of Science, Research and the Arts
- Elite Network of Bavaria (ENB) Macromolecular Sciences
The photophysical properties of films of alkyl-substituted polythiophenes are governed by a subtle interplay between intra- and interchain electronic couplings. The intramolecular properties, however, are still not entirely clear because polythiophenes possess a strong tendency to form,r-stacked aggregate structures with appreciable interchain couplings. Here we employ low-temperature single-molecule photoluminescence spectroscopy on isolated regioregular poly(3-hexylthiophene), P3HT, chains with different, but well-defined molecular weights to reveal the intrachain properties of their emitting sites. We find that the inhomogeneous distribution function of the zero-phonon lines (ZPL) is very narrow (<480 cm(-1), 60 meV), which indicates a low degree of torsional disorder of the P3HT backbone on length scales of the emitting sites (despite a large mean dihedral angle). Moreover, the single chain ZPLs are exclusively located in the high energy tail of the corresponding spectrum of a disordered ensemble. Using concentration-dependent measurements in combination with time-dependent density functional theory, we show that this spectral shift stems from aggregation-induced partial planarization and concomitant electronic coupling between segments of neighboring P3HT chains.
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