Selective Orbital Imaging of Excited States with X-Ray Spectroscopy: The Example of α-MnS

• Main Authors: A. Amorese, B. Leedahl, M. Sundermann, H. Gretarsson, Z. Hu, H.-J. Lin, C. T. Chen, M. Schmidt, H. Borrmann, Yu. Grin, A. Severing, M. W. Haverkort, L. H. Tjeng
• Format: Article
• Language: English
• Published: American Physical Society 2021-01-01
• Series: Physical Review X
• Online Access: http://doi.org/10.1103/PhysRevX.11.011002

Herein we show that nonresonant inelastic x-ray scattering involving an s core level is a powerful spectroscopic method to characterize the excited states of transition metal compounds. The spherical charge distribution of the s core hole allows the orientational dependence of the intensities of the various spectral features to produce a spatial charge image of the associated multiplet states in a straightforward manner, thereby facilitating the identification of their orbital character. In addition, the s core hole does not add an extra orbital angular momentum component to the multiplet structure so that the well-established Sugano-Tanabe-Kamimura diagrams can be used for the analysis of the spectra. For α-MnS we observe the spherical charge density corresponding to its high-spin 3d^{5} (^{6}A_{1}) ground state configuration and we were able to selectively image its excited states and identify them as t_{2g} (^{5}T_{2}) and e_{g} (^{5}E) with an energy splitting 10Dq of 0.78 eV.