Photo-induced phase transition on black samarium monosulfide

Abstract

To investigate the role of the excitons for the origin of the pressure-induced phase transition (BGT) from the black-colored insulator (BI) to the golden-yellow-colored metal (GM) of samarium monosulfide (SmS), optical reflectivity, Sm $3d$ X-ray absorption spectroscopy (XAS), and X-ray diffraction (XRD) with the creation of excitons by photoexcitation (PE) are reported. In the pump-probe reflectivity measurement, following a huge reflectivity change of about 22 %, three different relaxation times with a vibration component were observed. The fast component with the relaxation time ($\tau$) of less than 1 ps is due to the excitation and relaxation of electrons into the conduction band, and the slowest one with $\tau > {\rm several} 100$ ps originates from the appearance of the photo-induced (PI) state. The components with $\tau \sim 10$ ps and vibration originate from the appearance of the PI state and the interference between the reflection lights at the sample surface and the boundary between the BI and PI states, suggesting that the electronic structure of the PI phase is different from that of the BI state. XAS spectra indicate that the Sm mean valence is shifted from the Sm$^{2+}$ dominant to the intermediate between Sm$^{2+}$ and Sm$^{3+}$ by PE but did not change to that of the GM phase across BGT, consistent with the reflectivity data. The XRD result after PE shows that the PI state has much less lattice contraction than the GM phase. These results suggest that the BGT cannot be achieved solely by creating excitons after PE but requires other effects, such as a lattice contraction.