Probing the spectral dynamics of single terrylenediimide molecules in low-temperature solids

Abstract Fluorescence excitation lines of single terrylenediimide (TDI) molecules were recorded in the matrices polyethylene (PE) and hexadecane (HD) in the temperature range between 1.4 and 13 K. From line width distributions at 2.5 K in both matrices it was concluded that the disorder, theoretically modeled by a distribution of two-level systems (TLSs), is about three times stronger in PE. Temperature-dependent measurements of the line shape of single chromophores showed a reversible broadening and shift of the zero-phonon lines. We attributed this behavior to dephasing caused by pseudolocal phonons and to spectral diffusion caused by fluctuating TLSs of the disordered host. Following the…