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Register a new userSurface properties of SmB6 from x-ray photoelectron spectroscopy
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N. Heming
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We have investigated the properties of cleaved SmB$_6$ single crystals by x-ray photoelectron spectroscopy. At low temperatures and freshly cleaved samples a surface core level shift is observed which vanishes when the temperature is increased. A Sm valence between 2.5 - 2.6 is derived from the relative intensities of the Sm$^{2+}$ and Sm$^{3+}$ multiplets. The B/Sm intensity ratio obtained from the core levels is always larger than the stoichiometric value. Possible reasons for this deviation are discussed. The B $1s$ signal shows an unexpected complexity: an anomalous low energy component appears with increasing temperature and is assigned to the formation of a suboxide at the surface. While several interesting intrinsic and extrinsic properties of the SmB$_6$ surface are elucidated in this manuscript no clear indication of a trivial mechanism for the prominent surface conductivity is found.
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We have carried out bulk-sensitive hard x-ray photoelectron spectroscopy (HAXPES) measurements on in-situ cleaved and ex-situ polished SmB6 single crystals. Using the multiplet-structure in the Sm 3d core level spectra, we determined reliably that the valence of Sm in bulk SmB6 is close to 2.55 at ~5 K. Temperature dependent measurements revealed that the Sm valence gradually increases to 2.64 at 300 K. From a detailed line shape analysis we can clearly observe that not only the J=0 but also the J=1 state of the Sm 4f 6 configuration becomes occupied at elevated temperatures. Making use of the polarization dependence, we were able to identify and extract the Sm 4f spectral weight of the bulk material. Finally, we revealed that the oxidized or chemically damaged surface region of the ex-situ polished SmB6 single crystal is surprisingly thin, about 1 nm only.
Samarium hexaboride crystallizes in a simple cubic structure (space group #221, Pm-3m), but its properties are far from being straightforward. Initially classified as a Kondo insulator born out of its intriguing intermediate valence ground state, SmB6 has been recently predicted to be a strongly correlated topological insulator. The subsequent experimental discovery of surface states has revived the interest in SmB6, and our purpose here is to review the extensive and in many aspects perplexing experimental record of this material. We will discuss both surface and bulk properties of SmB6 with an emphasis on the role of crystal growth and sample preparation. We will also highlight the remaining mysteries and open questions in the field.
A laboratory hard X-ray photoelectron spectroscopy (HXPS) system equipped with a monochromatic Cr K$alpha$ ($h u = 5414.7$ eV) X-ray source was applied to an investigation of the core-level electronic structure of La$_{1-x}$Sr$_x$MnO$_3$. No appreciable high binding-energy shoulder in the O $1s$ HXPS spectra were observed while an enhanced low binding-energy shoulder structure in the Mn $2p_{3/2}$ HXPS spectra were observed, both of which are manifestation of high bulk sensitivity. Such high bulk sensitivity enabled us to track the Mn $2p_{3/2}$ shoulder structure in the full range of $x$, giving us a new insight into the binding-energy shift of the Mn $2p_{3/2}$ core level. Comparisons with the results using the conventional laboratory XPS ($h u = 1486.6$ eV) as well as those using a synchrotron radiation source ($h u = 7939.9$ eV) demonstrate that HXPS is a powerful and convenient tool to analyze the bulk electronic structure of a host of different compounds.
This Comment demonstrates that a comparison analysis by Seah and Gilmore between experimental data on the X-ray photoelectron spectroscopy intensities and theoretical data by Trzhaskovskaya et al. is misleading due to a number of serious errors made by Seah and Gilmore (Phys. Rev. B, 73, 174113).
Undoped and slightly Eu-doped SmB6 show the opening of a gap with decreasing temperature below ~150 K. The spectral shapes near the Fermi level (EF) at 15 K have shown strong increase in intensity of a peak at a binding energy (EB) of around 12 meV with decreasing the photon energy (hn) from 17 eV down to 7 eV. Angle resolved spectra of SmB6 measured at hn = 35 eV just after the in-situ cleavage showed clear dispersions of several bands in the EB region from EF to 4 eV. Spin-polarized photoelectron spectra were then measured at 12 K and light incidence angle of ~50 deg. In contrast to the lack of spin polarization for the linearly polarized light excitation, clear spin polarization was observed in the case of circularly polarized light excitation. The two prominent peaks at EB~12 and ~150 meV have shown opposite signs of spin polarization which are reversed when the helicity of the light is reversed. The sign and the magnitude of spin- polarization are consistent with a theoretical prediction for the 6H5/2 and 6H7/2 states.
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