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We study the excitonic coupling and homogeneous spectral line width of bricklayer J-aggregate films. We begin by analysing the structural informationrevealed by the two-exciton states probed in two-dimensional spectra. Our firstmain result is that the relation between the excitonic couplings and thespectral shift in a two-dimensional structure is different (larger shift forthe same nearest neighbour coupling) from that in a one-dimensional structure,which leads to an estimation of dipolar coupling in two-dimensional lattices.We next investigate the mechanisms of homogeneous broadening - populationrelaxation and pure dephasing - and evaluate their relative importance inlinear and two-dimensional aggregates. Our second main result is that puredephasing dominates the line width in two-dimensional systems up to a crossovertemperature, which explains the linear temperature dependence of thehomogeneous line width. This is directly related to the decreased density ofstates at the band edge when compared with linear aggregates, thus reducing thecontribution of population relaxation to dephasing. Pump-probe experiments aresuggested to directly measure the lifetime of the bright state and cantherefore support the proposed model.

How two-dimensional brick layer J-aggregates differ from linear ones: excitonic properties and line broadening mechanisms