Spin-Boson Hamiltonian and Optical Absorption of Molecular Dimers

Abstract

An analysis of the eigenstates of a symmetry-broken spin-boson Hamiltonian is performed by computing Bloch and Husimi projections. The eigenstate analysis is combined with the calculation of absorption bands of asymmetric dimer configurations constituted by monomers with nonidentical excitation energies and optical transition matrix elements. Absorption bands with regular and irregular fine structures are obtained and related to the transition from the coexistence to a mixing of adiabatic branches in the spectrum. It is shown that correlations between spin states allow for an interpolation between absorption bands for different optical asymmetries.