Are the spectral trails of single molecules consistent with the standard two-level system model of glasses at low temperatures? Original Research Article

The spectral trail of a single molecule is a 2D plot of many repeated spectra displayed as a function of time. Here, we present an analysis of the spectral trails of some 70 terrylene molecules in polymers. We compare the features of individual trails to the standard model of two-level systems (TLSs) in glasses at low temperatures, and we find a good overall agreement for a majority of molecules. However, more than 30% of the molecular trails cannot be reconciled with the standard model. For example, we found three-level systems, evidence for a strong coupling between some TLSs, and spectral drifts. Whereas our data confirm that the standard TLS model describes large ensembles of TLSs quite satisfactorily, this may result only from a cancellation of the deviations. Therefore, the application of the model to explain the spectral diffusion of individual molecules must be questioned in each particular case.