Optically induced softening of the charge-transfer gap in Sr2CuO2Cl2

Abstract

Energy- and time-resolved spectroscopy reveals a photoinduced softening of the charge-transfer gap in the insulating copper oxide Sr2CuO2Cl2 that indicates rapid and efficient photoproduction of optical phonons. By relating the pump-probe signal amplitude to the thermal difference spectrum, we estimate that eleven to twenty optical phonons are created for every one 3 eV photon. Assuming relaxation to the optical absorption edge at 1.5 eV, this corresponds to 70-130 meV per boson. While the lower limit is consistent with relaxation exclusively through optical phonons, the upper limit suggests a significant role for magnetic excitations. We observe a photoinduced bleaching of the gap excitation that we associate with phase space filling, and estimate the excluded area of the photoexcited state to be about nine copper oxide plaquettes. The temporal decay of the pump-probe signal is consistent with anharmonic phonon decay.