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Evolution of the electronic structure across the filling-control and bandwidth-control metal-insulator transitions in pyrochlore-type Ru oxides

Okamoto, Jun*; Fujimori, Shinichi   ; Okane, Tetsuo  ; Fujimori, Atsushi*; Abbate, M.*; Yoshii, Shunsuke*; Sato, Masatoshi*

We have performed photoemission and soft X-ray absorption studies of pyrochlore-type Ru oxides, namely, the filling-control system Sm$$_{2-x}$$Ca$$_x$$Ru$$_2$$O$$_7$$ and the bandwidth-control system Sm$$_{2-x}$$Bi$$_x$$Ru$$_2$$O$$_7$$, which show insulator-to-metal transition with increasing Ca and Bi concentration, respectively. Core levels and the O 2$$p$$ valence band in Sm$$_{2-x}$$Ca$$_x$$Ru$$_2$$O$$_7$$ show almost the same amount of monotonous upward energy shifts with Ca concentration, which indicates that the chemical potential is shifted downward due to hole doping. The Ru 4$$d$$ band in Sm$$_{2-x}$$Ca$$_x$$Ru$$_2$$O$$_7$$ is also shifted toward the Fermi level ($$E_F$$) with hole doping and the density of states (DOS) at $$E_F$$ increases. The core levels in Sm$$_{2-x}$$Bi$$_x$$Ru$$_2$$O$$_7$$, on the other hand, do not show clear energy shifts except for the Ru 3$$d$$ core level, whose line shape change also reflects the increase of metallic screening with Bi concentration. We observe pronounced spectral weight transfer from the incoherent to the coherent parts of the Ru $$4d$$ $$t_{2g}$$ band with Bi concentration, which is expected for a bandwidth-control Mott-Hubbard system. The increase of the DOS at $$E_F$$ is more abrupt in the bandwidth-control Sm$$_{2-x}$$Bi$$_x$$Ru$$_2$$O$$_7$$ than in the filling-control Sm$$_{2-x}$$Ca$$_x$$Ru$$_2$$O$$_7$$, in accordance with a recent theoretical prediction. Effects of charge transfer between the Bi 6$$sp$$ band and the Ru 4$$d$$ band are also discussed.



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Category:Materials Science, Multidisciplinary



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