Dispersive hole growth kinetics and fluence broadening of the zero-phonon hole of impurities in amorphous hosts

Abstract

Abstract A detailed treatment of the relationship between the dispersive growth kinetics of the zero-phonon hole (ZPH) of an impurity molecule in an amorphous host and burn fluence broadening of the ZPH is presented. Focus is on non-photochemical hole burning (NPHB). The equation used for simulations accounts for dispersion due to a distribution of tunneling parameters (λ-distribution), the angle between the laser polarization and the transition dipole (α-distribution), and off-resonant absorption of the zero-phonon line (ω-distribution). Two cases are considered: burned laser linewidth narrow relative to the homogeneous width of the zero-phonon line; and the reverse situation. Results are presented for two model systems whose parameter values are similar to those of aluminum phthalocyanine tetrasulphonate (APT) in hyperquenched glassy water and in hyperquenched glassy ethanol. For comparison, results are presented for the case where the hole growth kinetics are non-dispersive (single-exponential). It is found that at the early stage of burning fluence broadening is considerably more severe for a dispersive system than for a non-dispersive system. A straightforward explanation for this is given. The results are compared with those of earlier works on dispersive hole growth kinetics and fluence broadening. The results reveal the types of experiment needed to understand the aforementioned relationship, a requirement for determination of the homogeneous width of the ZPH that reflects the dynamics of the system.