Collective Effects in Linear Spectroscopy of Molecular Aggregates

A consistent analysis of linear spectroscopy for arrays of dipole-coupled two-level molecules reveals distinct signatures of weak and strong coupling regimes separated by a critical point. Multiple molecular excitations (odd(even) in weak(strong) coupling) are accessed from the ground state. As the coupling increases, the single excitation oscillator strength rapidly exceeds the Heitler-London value and diverges at the critical point, returning to a quadratic size scaling in strong coupling, where also the photon frequency decreases with size. The lowest accessible excitation is found to show a one-photon hyperradiance.