- Accepted Paper
Two-exciton bound states in the Merrifield exciton model
Phys. Rev. B - Accepted 5 October, 2026
DOI: https://doi.org/10.1103/9c6b-gk9f
Phys. Rev. B - Accepted 5 October, 2026
DOI: https://doi.org/10.1103/9c6b-gk9f
Understanding the formation and dynamics of two-exciton bound states (BSs) is crucial for harnessing multi-exciton phenomena and designing next-generation organic semiconductor materials. While various mechanisms such as intermolecular exciton-exciton interactions or multi-level intramolecular configurations can generate these BSs, a fundamental understanding of their underlying lattice dynamics remains a key challenge. Within this context, the Merrifield exciton model stands out as a premier framework for capturing the intricate quantum mixing between single-site doubly-excited states and two-particle scattering continuum. In this work, by constructing a set of exact two-exciton Bloch states and applying a plane-wave ansatz to treat the resulting inhomogeneous tridiagonal matrices, we provide a complete, rigorous solution to the two-exciton problem in a finite-size Merrifield chain. We analytically map the parameter regions that support two-exciton BSs, proving that at most two distinct types of BSs can emerge, located either above or below the scattering continuum. Furthermore, we provide a quantitative interpretation of how these two types of BSs evolve as a function of the total wave number within the whole Brillouin zone. The obtained closed-form expressions for the eigenenergies and wave functions offer valuable benchmarks for exploring exciton dynamics and optical responses in related molecular aggregates.
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