下地幔压力条件下（Mg0.97，Fe0.03）O方镁铁矿的光学性质∗

摘要

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.%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.