Pressure induced spin transition revealed by iron M2,3-edge spectroscopy

Nyrow, Alexander; Tse, John S.; Hiraoka, Nozomu; Desgreniers, Serge; Büning, Thomas; Mende, Kolja; Tolan, Metin; Wilke, Max; Sternemann, Christian

doi:10.1063/1.4886971

Cited by 18 publications

(12 citation statements)

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“…As the scattering vector becomes larger, the octupole transition become dominant and the dipole transition becomes subordinate; the intensity around the transferred energy 53 ∼ 55 eV become intense and the intensity above 55 eV becomes weak. A similar tendency can be seen in the XRS spectra on iron oxides 10. In order to compare the observation and the calculation, we naively assume that the lifetime broadening is Γ = max (0.1E + 0.14, 0.14) eV, where E is the relative transferred…”

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Magnetic circular dichroism in hard x-ray Raman scattering as a probe of local spin polarization

Takahashi

Hiraoka

2019

Phys. Rev. B

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We argue that the magnetic circular dichroism (MCD) of the hard x-ray Raman scattering (XRS) could be used as an element selective probe of local spin polarization. The magnitude of the XRS-MCD signal is directly proportional to the local spin polarization when the angle between the incident wavevector and the magnetization vector is 135 • or −45 • . By comparing the experimental observation and the configuration interaction calculation at the L 2,3 and M 2,3 edges of ferromagnetic iron, we suggest that the integrated MCD signal in terms of the transferred energy could be used to estimate the local spin moment even in the case where the application of the spin sum-rule in X-ray absorption is questionable. We also point out that XRS-MCD signal could be observed at the M 1 edge with a magnitude comparable to that at the M 2,3 edge, although the spin-orbit coupling is absent in the core orbital. By combining the XRS-MCD at various edges, spin polarization distribution depending on the orbital magnetic quantum number would be determined.1 arXiv:1909.13490v1 [cond-mat.mtrl-sci] 30 Sep 2019 X-ray magnetic circular dichroism (MCD) has been one of the powerful tools to investigate the electronic structure in magnetic materials. Particularly, owing to the orbital and spin sum-rules, 1,2 the MCD in the soft x-ray absorption spectroscopy (XAS) has been playing crucial roles for elucidating the electronic structure at and around the absorption site. 3 The MCD measurements in x-ray emission and resonant inelastic scattering are also important tools to clarify the electronic excitations in magnetic materials. 4Recently, the MCD in the hard x-ray Raman scattering (XRS) at the Fe L 2,3 -edges in the ferromagnetic iron has been investigated. 5,6 The XRS is a kind of non-resonant inelasticx-ray scattering. 7 In the process of photon scattering, where an incident photon of energy ω i is absorbed and a photon of energy ω f is emitted, the electron system in the initial ground state of the energy E i is excited to the final state of the energyThe final state of the XRS is essentially the same with that of XAS: A core hole is left behind at the scattering site and an electron is added to the valence or conduction state.Therefore, the XRS intensity as a function of transferred energy is similar to the soft xray absorption coefficient as a function of the incident photon energy. Contrasting to the XAS, the hard-in-hard-out feature of the XRS is preferable for bulk sensitive measurements or the measurements under extreme conditions. In addition, the XRS can access the final states that are inaccessible by the dipole transition, because the non-dipole transition matrix elements become significant for shallow core excitation. By virtue of these features, the innercore-exciting XRS has been demonstrating its usefulness particularly to unveil the electronic state of materials under extreme conditions. 8 Recently, the electronic state of Fe in Fe 2 SiO 4 , Fe 2 O 3 and FeS under high pressure is discussed by analyzing the XRS spectra at the F...

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Magnetic circular dichroism in hard x-ray Raman scattering as a probe of local spin polarization

Takahashi

Hiraoka

2019

Phys. Rev. B

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“…As shown by Nyrow et al . 40 the spin transition pressure and spin transition range can be characterized by the integral of the absolute value of A ( p ), which is given by the differences between spectra measured at certain pressure p and a HS reference measured at ambient conditions or low pressure. As our siderite reference, here we use the M 2,3 -edge and L 2,3 -edge measured at ambient conditions and 2.4 GPa, respectively.…”

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confidence: 99%

“…In this work we exploit x-ray Raman scattering (XRS) spectroscopy to study the iron M 2,3 -edges 40 and L 2,3 -edges 41 of siderite and magnesiosiderite in situ at high pressure in a diamond anvil cell (DAC) in order to probe the electronic structure of iron. XAS measurements at the iron L 2,3 -edges (2p→3d) for light- or temperature induced spin transitions have shown that the L 2,3 -edge is highly sensitive to the spin state 42 , 43 , but high pressure experiments using DAC prevent the use of soft x-ray absorption for the in situ study of the L 2,3 - and/or M 2,3 -edges of iron in the carbonates due to the strong absorption of soft x-rays by the diamond anvils.…”

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confidence: 99%

“…Lately, Nyrow et al . 40 demonstrated the sensitivity of XRS with respect to the spin state by measuring the iron M 2,3 -edge of FeS powder at high pressure. In this study we investigate the pressure-induced HS to LS transition of synthetic siderite and magnesiosiderite single crystals at the iron M 2,3 -edge and iron L 2,3 -edge in the pressure range up to 57 GPa using argon and helium as pressure medium at room temperature by means of XRS.…”

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Pressure driven spin transition in siderite and magnesiosiderite single crystals

Weis

Sternemann

Cerantola

et al. 2017

Sci Rep

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Iron-bearing carbonates are candidate phases for carbon storage in the deep Earth and may play an important role for the Earth’s carbon cycle. To elucidate the properties of carbonates at conditions of the deep Earth, we investigated the pressure driven magnetic high spin to low spin transition of synthetic siderite FeCO3 and magnesiosiderite (Mg0.74Fe0.26)CO3 single crystals for pressures up to 57 GPa using diamond anvil cells and x-ray Raman scattering spectroscopy to directly probe the iron 3d electron configuration. An extremely sharp transition for siderite single crystal occurs at a notably low pressure of 40.4 ± 0.1 GPa with a transition width of 0.7 GPa when using the very soft pressure medium helium. In contrast, we observe a broadening of the transition width to 4.4 GPa for siderite with a surprising additional shift of the transition pressure to 44.3 ± 0.4 GPa when argon is used as pressure medium. The difference is assigned to larger pressure gradients in case of argon. For magnesiosiderite loaded with argon, the transition occurs at 44.8 ± 0.8 GPa showing similar width as siderite. Hence, no compositional effect on the spin transition pressure is observed. The spectra measured within the spin crossover regime indicate coexistence of regions of pure high- and low-spin configuration within the single crystal.

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“…[37][38][39][40][41][42][43] Recently, in situ high pressure measurements of the Fe M 2/3 -edge demonstrated the ability to track the pressure induced spin cross-over in FeS and to extract quantitative information about the crystal eld splitting of the 3d states in iron. 44 The Fe M 2/3 -edge is signicantly modied by weak changes of the oxidation and spin state, but it is less sensitive to the local coordination. 45 Recently, magnetic circular dichroism of X-ray Raman scattering was observed at the iron L 2/3 -edge of pure iron.…”

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confidence: 99%

Bulk sensitive determination of the Fe³⁺/Fe_Tot-ratio in minerals by Fe L_2/3-edge X-ray Raman scattering

Nyrow

Sternemann

Tse

et al. 2016

J. Anal. At. Spectrom.

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Pressure induced spin transition revealed by iron M2,3-edge spectroscopy

Cited by 18 publications

References 31 publications

Magnetic circular dichroism in hard x-ray Raman scattering as a probe of local spin polarization

Magnetic circular dichroism in hard x-ray Raman scattering as a probe of local spin polarization

Pressure driven spin transition in siderite and magnesiosiderite single crystals

Bulk sensitive determination of the Fe³⁺/Fe_Tot-ratio in minerals by Fe L_2/3-edge X-ray Raman scattering

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Pressure induced spin transition revealed by iron M2,3-edge spectroscopy

Cited by 18 publications

References 31 publications

Magnetic circular dichroism in hard x-ray Raman scattering as a probe of local spin polarization

Magnetic circular dichroism in hard x-ray Raman scattering as a probe of local spin polarization

Pressure driven spin transition in siderite and magnesiosiderite single crystals

Bulk sensitive determination of the Fe3+/FeTot-ratio in minerals by Fe L2/3-edge X-ray Raman scattering

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Bulk sensitive determination of the Fe³⁺/Fe_Tot-ratio in minerals by Fe L_2/3-edge X-ray Raman scattering