Aluminum-bearing minerals show different hydrogen evolution and dissolution properties when subjected to radiation, but the complicated sequence of events following interaction with high-energy radiation is not understood. To gain insight into the possible mechanisms of hydrogen production in nanoparticulate minerals, we study the electronic response and determine the bandgap energies of three common aluminum-bearing minerals with varying hydrogen content: gibbsite (Al(OH)₃), boehmite (AlOOH), and alumina (Al₂O₃) using electron energy loss spectroscopy, X-ray photoelectron spectroscopy, and first-principles electronic structure calculations employing hybrid density functionals. We find that the amount of hydrogen has only a small effect on the number and spectrum of photoexcitations in this class of materials. Electronic structure calculations demonstrate that low energy electrons are isotropically mobile, while holes in the valence band are likely constrained to move in layers. Furthermore, holes in the valence band of boehmite are found to be significantly more mobile than those in gibbsite, suggesting that the differences in radiolytic and dissolution behavior are related to hole transport.

中文翻译：

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含铝矿物的电子响应

含铝矿物在受到辐射时会表现出不同的氢释放和溶解特性，但与高能辐射相互作用后的复杂事件序列尚不清楚。为了深入了解纳米颗粒矿物中产氢的可能机理，我们研究了电子响应并确定了三种氢含量不同的常见含铝矿物的带隙能：三水铝石（Al（OH）₃），勃姆石（AlOOH），和氧化铝（Al ₂ O ₃），使用电子能量损失谱，X射线光电子能谱和采用混合密度泛函的第一性原理电子结构计算。我们发现，在这类材料中，氢的含量对光激发的数量和光谱只有很小的影响。电子结构计算表明，低能电子是各向同性运动的，而价带中的空穴可能会受到限制而分层移动。此外，发现勃姆石价带中的空穴比三水铝石中的空穴更具流动性，这表明辐射分解和溶解行为的差异与空穴的运输有关。