Flh. Brown et Rj. Silbey, AN INVESTIGATION OF THE EFFECTS OF 2-LEVEL SYSTEM COUPLING ON SINGLE-MOLECULE LINESHAPES IN LOW-TEMPERATURE GLASSES, The Journal of chemical physics, 108(17), 1998, pp. 7434-7450
A theoretical framework for determining the lineshapes of single molec
ules in low temperature glasses is presented. Our methods, in contrast
to previous efforts, include coupling between two level systems (TLSs
). This framework is applied to the physical system consisting of the
chromophore terrylene embedded in the amorphous host polystyrene. We a
nalyze the effect of TLS-TLS coupling on both individual lineshapes an
d linewidth histograms. Ourresults indicate that, although TLS-TLS cou
pling is certainly capable of producing noticeable changes in individu
al spectral lines relative to the uncoupled results, linewidth histogr
ams are relatively unaffected by said coupling. An interpretation of t
his result is suggested. (C) 1998 American Institute of physics.