Spin and valence states of iron in Al-bearing silicate glass at high pressures studied by synchrotron Mossbauer and X-ray emission spectroscopy
文献类型：期刊论文
| 作者 | Mao, Z ; Lin, JF ; Yang, J ; Wu, JJ ; Watson, HC ; Xiao, YM ; Chow, P ; Zhao, JY |
| 刊名 | AMERICAN MINERALOGIST
 |
| 出版日期 | 2014 |
| 卷号 | 99期号:2-3页码:415 |
| 关键词 | Silicate glass high pressure synchrotron Mossbauer spectroscopy X-ray emission spectroscopy lower mantle |
| ISSN号 | 0003-004X |
| 通讯作者 | Mao, Z (reprint author), Univ Texas Austin, Dept Geol Sci, Jackson Sch Geosci, Austin, TX 78712 USA. |
| 中文摘要 | High-pressure synchrotron Mossbauer (SMS) and X-ray emission (XES) spectroscopic measurements were conducted to investigate the spin and valence states of iron in (A1,Fe)-bearing magnesium silicate glass (Mg0.79Fe0.10Al0.10Si0.96O3) up to 126 GPa and 300 K. By analyzing the Fe K beta emission spectra using the integrated relative difference (IRD) method, which accounts for the spectral broadening effects, the derived total spin momentum (S) of the iron in the glass shows no observable changes with pressure within the experimental uncertainties. A two-doublet fitting model representing two diverse local iron atomic environments was used to satisfactorily simulate the high-pressure SMS spectra of iron in the glass. The doublet with an averaged quadrupole splitting (QS) value of 1.94(+/- 0.25) mm/s and chemical shift (CS) of 1.02(+/- 0.25) minis at ambient conditions was assigned to be high-spin Fe2+, whereas the second doublet with QS = 0.83(+/- 0.25) mm/s and CS = 0.49(+/- 0.25) mm/s was assigned to be high-spin Fe3+. Increasing pressure continuously elevates the QS of Fe2+ from similar to 2 mm/s at ambient pressure to 3.5 mm/s at 126 GPa, while Fe3+ only exhibits a slight increase in the QS to 1.34(+/- 0.25) mm/s. Comparing with previous experimental and theoretical studies on the local geometries and hyperfine parameters of silicate glasses and minerals, we conclude that the occurrence of the extremely high QS of Fe2+ in our glass above similar to 40-50 GPa can be associated with the enhanced density and diverse distortions and geometries of the local Fe2+ environments. Our combined XES and SMS results show that both Fe2+ and Fe3+ ions in Al-bearing silicate remain in the high-spin state, rather than undergoing a spin-pairing transition as proposed previously. Assuming that the silicate glass results can be used as an analog for understanding silicate melts, our results here indicate that iron ions likely experience significant changes in the local environments yet remain overall in the high-spin state in silicate melts at the extreme pressure and temperature conditions of the deep mantle. |
| 资助信息 | U.S. National Science Foundation [EAR-1053446, EAR-1056670]; Carnegie/DOE Alliance Center (CDAC); DOE-NNSA [DE-NA0001974]; DOE-BES [DE-FG02-99ER45775, DE-AC02-06CH11357]; NSF |
| 语种 | 英语 |
| 公开日期 | 2015-04-14 |
| 源URL | [http://ir.iphy.ac.cn/handle/311004/58852]  |
| 专题 | 物理研究所_物理所公开发表论文_物理所公开发表论文_期刊论文 |
| 推荐引用方式 GB/T 7714 | Mao, Z,Lin, JF,Yang, J,et al. Spin and valence states of iron in Al-bearing silicate glass at high pressures studied by synchrotron Mossbauer and X-ray emission spectroscopy[J]. AMERICAN MINERALOGIST,2014,99(2-3):415. |
| APA | Mao, Z.,Lin, JF.,Yang, J.,Wu, JJ.,Watson, HC.,...&Zhao, JY.(2014).Spin and valence states of iron in Al-bearing silicate glass at high pressures studied by synchrotron Mossbauer and X-ray emission spectroscopy.AMERICAN MINERALOGIST,99(2-3),415. |
| MLA | Mao, Z,et al."Spin and valence states of iron in Al-bearing silicate glass at high pressures studied by synchrotron Mossbauer and X-ray emission spectroscopy".AMERICAN MINERALOGIST 99.2-3(2014):415. |
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来源：物理研究所
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