Unveiling Multiquantum Excitonic Correlations in Push-Pull Polymer Semiconductors.

ABSTRACT: Bound and unbound Frenkel-exciton pairs are essential transient precursors for a variety of photophysical and biochemical processes. In this work, we identify bound and unbound Frenkel-exciton complexes in an electron push-pull polymer semiconductor using coherent two-dimensional spectroscopy. We find that the dominant A_0-1 peak of the absorption vibronic progression is accompanied by a subpeak, each dressed by distinct vibrational modes. By considering the Liouville pathways within a two-exciton model, the imbalanced cross-peaks in one-quantum rephasing and nonrephasing spectra can be accounted for by the presence of pure biexcitons. The two-quantum nonrephasing spectra provide direct evidence for unbound exciton pairs and biexcitons with dominantly attractive force. In additio

SUBMITTER: Zheng Y 

PROVIDER: S-EPMC11017317 | biostudies-literature | 2024 Apr

REPOSITORIES: biostudies-literature