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本文采用第一性原理方法, 计算了(Mg0.97, Fe0.03) O方镁铁矿的理想晶体和含镁-氧离子双空位点缺陷晶体在下地幔压力条件下的光学性质. 吸收光谱数据表明, 方镁铁矿理想晶体的结果与晶体场等理论预测的结果相似:压力诱导铁自旋态的转变将导致方镁铁矿吸收谱有巨大蓝移, 并在近红外光区出现了透明现象. 然而, 在方镁铁矿中含有点缺陷时, 其结果与晶体场等理论预测结果存在本质差异:铁自旋态的转变将导致在近红外光区的吸收性显著增强. 含点缺陷晶体折射率的计算结果表明, 压力、波数及铁自旋态的转变对(Mg0.97, Fe0.03) O方镁铁矿的折射率有较明显地影响. 本文结果不仅对探索下地幔方镁铁矿在高压下的光学性质有重要的参考价值, 而且还指明高压吸收光谱的测量可能是准确获得铁自旋态信息一个好的手段.The optical-absorption and refractive-index properties of (Mg0.97, Fe0.03)O ferropericlase crystals without and with Mg and O ionic divacancy point-defect under the pressure of the Earth’s lower mantle are investigated using the first-principles calculations. Optical-absorption data show that the perfect-crystal results are similar to the predictions from the crystal-field theory:the pressure-induced spin transition of iron in ferropericlase causes a large blue-shift in its optical-absorption spectrum, leaving the near-infrared region transparent. However, when there are point defects in ferropericlase, the calculated optical-absorption results are completely inconsistent with predictions from the crystal-field theory, the spin transition causes the enhancement in the optical absorption in the near-infrared region. Refractive-index data of defect crystal indicate that the effects of pressure, wavenumber, and spin-transition on the high-pressure refractive-index of (Mg0.97, Fe0.03)O ferropericlase are obvious, but perfect-crystal results show that those effects should be relatively weak. The ～15%-20% iron-bearing ferropericlase is currently considered as an important mineral in the Earth’s lower mantle. Due to similar characteristics of the observed high-pressure optical-absorption spectrum in ferropericlase with different iron content, we suggest that:(1) the above-mentioned calculated results is conducive to the understanding of high-pressure optical properties of lower-mantle ferropericlase and the exploring of the origin of discrepancies in its high-pressure optical-absorption spectrum between experiment and crystal-field theory; (2) the high-pressure optical-absorption spectrum measurements may be a good approach for probing iron spin state.
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Keywords:
- high pressure /
- first-principles calculations /
- optical properties /
- ferropericlase
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[1] Lin J F, Speziale S, Mao Z, Marquardt S 2013 Rev. Geophys. 51 244
[2] Ammann M W, Brodholt J P, Dobson D P 2011 Earth Planet. Sci. Lett. 302 393
[3] He L 2008 Ph. D. Dissertation (Chengdu:Southwest Jiaotong University) (in Chinese) [何林 2008 博士学位论文(成都:西南交通大学)]
[4] He L, Gong Z Z, Jing F Q 2008 Chin. Phys. Lett. 25 332
[5] Anderson D L 2004 科学通报 49 2025
[6] Goncharov A F, Struzhkin V V, Jacobsen S D 2006 Science 312 1205
[7] Goncharov A F, Struzhkin V V, Montoya J A, Kharlamova S, Kundargi R, Siebert J, Badro J, Antonangeli D, Ryerson F J, Mao W 2010 Phys. Earth Planet. Inter. 180 148
[8] Murakami M, Goncharov A F, Hirao N, Masuda R, Mitsui T, Thomas S M, Bina C R 2014 Nat. Commun. 5 5428
[9] Badro J, Rueff J P, Vanko G, Monaco G, Fiquet G, Guyot F 2004 Science 305 383
[10] Badro J, Fiquet G, Guyot F, Rueff J P, Struzhkin V V, Vanko G, Monacoet G 2003 Science 300 789
[11] Burns R G 1993 Mineralogical Applications of Crystal Field Theory (2nd ed) (Cambridge:Cambridge University Press) pp146-239
[12] Sherman D M 1991 J. Geophys. Res. 96 14299
[13] Keppler H, Kantor I, Dubrovinski L S 2007 Am. Miner. 92 433
[14] Keppler H, Dubrovinsky L S, Narygina O, Kantor I 2008 Science 322 1529
[15] Hofmeister A M 2005 J. Geodyn. 40 51
[16] He L, Tang M J, Zeng M F, Zhou X M, Zhu W J, Liu F S 2013 Physica B 410 137
[17] He L, Tang M J, Yin J, Zhou X M, Zhu W J, Liu F S, He D W 2012 Physica B 407 694
[18] He X, He L, Tang M J, Xu M 2011 Acta Phys. Sin. 60 026102 (in Chinese) [何旭, 何林, 唐明杰, 徐明 2011 60 026102]
[19] Lin J F, Struzhkin V V, Jacobsen S D, Hu M, Chow P, Kung J, Liu H, Mao H K, Hemley R J 2005 Nature 436 377
[20] Tsuchiya T, Wentzcovitch R M, da Silva C R S, de Gironcoli S 2006 Phys. Rev. Lett. 96 198501
[21] Zhang F W, Walker A M, Wright K, Gale J D 2010 J. Mater. Chem. 20 10445
[22] Van Orman J A, Fei Y W, Hauri E H, Wang J H 2003 Geophys. Res. Lett. 30 1056
[23] Karaki B B, Khanduja G 2006 Am. Mineral. 91 511
[24] He L, Tang M J, Fang Y, Jing F Q 2008 Europhys. Lett. 83 39001
[25] Zhou X M, Wang X S, Li S N, Li J, Li J B, Jing F Q 2007 Acta Phys. Sin. 56 4965 (in Chinese) [周显明, 汪小松, 李赛男, 李俊, 李加波, 经福谦 2007 56 4965]
[26] Li J, Zhou X M, Li J B 2008 Rev. Sci. Instrum. 79 123107
[27] Goncharov A F, Haugen B D, Struzhkin V V, Beck P, Jacobsen S D 2008 Nature 456 231
[28] Van Orman J A, Crispin K L 2010 Rev. Mineral. & Geochem. 72 757
[29] Segall M D, Lindan P J D, Probert M J, Pickard C J, Hasnip P J, Clark S J, Payne M C 2002 J. Phys. :Condens. Matter 14 2717
[30] Kohn W, Sham L 1965 Phys. Rev. A 140 1133
[31] Vanderbilt D 1990 Phys. Rev. B 41 7892
[32] Perdew J P, Burke K, Ernzerhof M 1996 Phys. Rev. Lett. 77 3865
[33] Bengtson A, Persson K, Morgan D 2008 Earth Planet. Sci. Lett. 265 535
[34] Wu D, Zhao J J, Tian H 2013 Acta Phys. Sin. 62 049101 (in Chinese) [吴迪, 赵纪军, 田华 2013 62 049101]
[35] Song C L, Yang Z H, Su T, Wang K K, Wang J, Liu Y, Han G R 2014 Chin. Phys. B 23 057101
[36] Fischer T H, Almlof J 1992 J. Phys. Chem. 96 9768
[37] Wu Z Q, Justo J F, Wentzcovitch R M 2013 Phys. Rev. Lett. 110 228501
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