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J Phys Chem B. 2013 Jul 11;117(27):8245-55. doi: 10.1021/jp404498u. Epub 2013 Jun 26.

Frequency modulated femtosecond stimulated Raman spectroscopy of ultrafast energy transfer in a donor-acceptor copolymer.

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  • 1Department of Chemistry, University of North Carolina at Chapel Hill, Chapel Hill, NC 27514, USA.


A Raman-pump frequency modulation scheme and an automated signal-processing algorithm are developed for improved collection of time-resolved femtosecond stimulated Raman spectra. Together, these two advancements remove the broad background signals endemic to FSRS measurements and retrieve signals with high sensitivity. We apply this frequency-modulated femtosecond stimulated Raman spectroscopy (FM-FSRS) to the characterization of ultrafast energy transport in a copolymer comprised of polystyrene linked oligo(phenylene-ethynylene) donor and thiophene-benzothiadiazole acceptor chromophores. After photoexcitation of the donor, ultrafast energy transfer is monitored by the decay of donor vibrational modes and simultaneous growth of acceptor modes. The FM-FSRS method shows clear advantages in signal-to-noise levels, mitigation of artifact features, and ease of data processing over the conventional FSRS technique.

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