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We studied the spectral dynamics of single fluorescent dye molecules embeddedin ultrathin films (5 - 100 nm) of the amorphous polymer polyisobutylene atcryogenic temperatures and its variation with film thickness. Noticeableportion of molecules in the ensemble show a behavior which is inconsistent withthe standard tunneling model: Their spectral lines are subject to irreversiblespectral jumps, continuous shifting, and abrupt chaotic changes of thelinewidth or jumping rate. In films thinner than 100 nm, the occurrence of"non-standard" spectral behavior increases with decreasing sample thickness atfixed excitation intensity. In addition, it also increases with laserintensity.

Low temperature spectral dynamics of single molecules in ultrathin polymer films