Journal
PHYSICAL REVIEW B
Volume 78, Issue 23, Pages -Publisher
AMER PHYSICAL SOC
DOI: 10.1103/PhysRevB.78.235109
Keywords
excited states; excitons; high-speed optical techniques; polymer films
Funding
- National Science Foundation [NSF-DMR-0705163]
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We develop a theory of the electronic structure and photophysics of interacting chains of pi-conjugated polymers to understand the differences between solutions and films. While photoexcitation generates only the intrachain exciton in solutions, the optical exciton as well as weakly allowed charge-transfer excitons are generated in films. We extend existing theories of the lowest polaron pair and charge-transfer excitons to obtain descriptions of the excited states of these interchain species, and we show that a significant fraction of ultrafast photoinduced absorptions in films originates from the lowest charge-transfer exciton. Our proposed mechanism explains the simultaneous observation of polaronlike-induced absorption features peculiar to films in ultrafast spectroscopy and the absence of mobile charge carriers as deduced from other experiments. We also show that there is a 1:1 correspondence between the essential states that describe the photophysics of single chains and of interacting chains that constitute thin films.
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