Ultrafast electronic state conversion at room temperature utilizing hidden state in cuprate ladder system.

Photo-control of material properties on femto- (10(-15)) and pico- (10(-12)) second timescales at room temperature has been a long-sought goal of materials science. Here we demonstrate a unique ultrafast conversion between the metallic and insulating state and the emergence of a hidden insulating state by tuning the carrier coherence in a wide temperature range in the two-leg ladder superconductor Sr(14-x)Ca(x)Cu24O41 through femtosecond time-resolved reflection spectroscopy. We also propose a theoretical scenario that can explain the experimental results. The calculations indicate that the holes injected by the ultrashort light reduce the coherence among the inherent hole pairs and result in suppression of conductivity, which is opposite to the conventional photocarrier-doping mechanism. By using trains of ultrashort laser pulses, we successively tune the carrier coherence to within 1 picosecond. Control of hole-pair coherence is shown to be a realistic strategy for tuning the electronic state on ultrafast timescales at room temperature.

Photoinduced charge-transfer process in rubidium manganese hexacyanoferrate probed by Raman spectroscopy.

The photoinduced charge-transfer process in Rb(0.94)Mn[Fe(CN)(6)](0.98).0.2H(2)O is investigated by observing the valence states of the metal ions by Raman spectroscopy. The sample in the high-temperature phase is irradiated at the ligand to metal, CN(-)-->Fe(III) and charge-transfer band (lambda=395 nm). The Fe(III)-CN-Mn(II) pair valence state corresponding to the high-temperature configuration is totally depleted after prolonged irradiation, and the Fe(II)-CN-Mn(III) pair valence state corresponding to the low-temperature configuration appears. In addition, two kinds of CN stretching modes, ascribed to Fe(II)-CN-Mn(II) and Fe(III)-CN-Mn(III) pair valence states, are found. The photoproduction process of each pair valence states is well reproduced by a kinetic model assuming a charge transfer from Mn(II) to Fe(III). During irradiation, continuous shifts of the Raman peaks are found and ascribed to a release of the strain due to the lattice mismatching between the high-temperature and the photoinduced phases. This behavior indicates that the photoinduced phase created locally in the high-temperature-phase lattice grows up to a photoinduced phase domain. The conversion efficiency is lowered with decreasing temperature, indicating the existence of an energy barrier. We propose a model, which can explain the existence of an energy barrier in the electronic excited state.