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MnNiO3 revisited with modern theoretical and experimental methods
The Journal of Chemical Physics ( IF 4.4 ) Pub Date : 2017-11-03 , DOI: 10.1063/1.5000847
Allison L. Dzubak 1 , Chandrima Mitra 1 , Michael Chance 1 , Stephen Kuhn 1 , Gerald E. Jellison 1 , Athena S. Sefat 1 , Jaron T. Krogel 1 , Fernando A. Reboredo 1
Affiliation  

MnNiO3 is a strongly correlated transition metal oxide that has recently been investigated theoretically for its potential application as an oxygen-evolution photocatalyst. However, there is no experimental report on critical quantities such as the band gap or bulk modulus. Recent theoretical predictions with standard functionals such as LDA+U and HSE show large discrepancies in the band gaps (about 1.23 eV), depending on the nature of the functional used. Hence there is clearly a need for an accurate quantitative prediction of the band gap to gauge its utility as a photocatalyst. In this work, we present a diffusion quantum Monte Carlo study of the bulk properties of MnNiO3 and revisit the synthesis and experimental properties of the compound. We predict quasiparticle band gaps of 2.0(5) eV and 3.8(6) eV for the majority and minority spin channels, respectively, and an equilibrium volume of 92.8 Å3, which compares well to the experimental value of 94.4 Å3. A bulk modulus of 217 GPa is predicted for MnNiO3. We rationalize the difficulty for the formation of ordered ilmenite-type structure with specific sites for Ni and Mn to be potentially due to the formation of antisite defects that form during synthesis, which ultimately affects the physical properties of MnNiO3.

中文翻译:

MnNiO 3用现代理论和实验方法再探

MnNiO 3是一种高度相关的过渡金属氧化物,最近已在理论上进行了研究,认为其潜力可作为氧气释放型光催化剂。然而,没有关于临界量如带隙或体积模量的实验报告。对标准功能(例如LDA + U和HSE)的最新理论预测表明,根据所使用功能的性质,带隙中的差异较大(约1.23 eV)。因此,显然需要对带隙进行准确的定量预测,以评估其作为光催化剂的效用。在这项工作中,我们提出了MnNiO 3的整体性质的扩散量子蒙特卡罗研究。并重新研究了该化合物的合成和实验性质。我们预测的2.0(5)eV和3.8(6)电子伏特为广大和少数自旋通道,分别准粒子的带隙,以及平衡量的92.8埃3,其比较很好地为94.4埃的实验值3。MnNiO 3的体积模量预计为217 GPa 。我们合理化了难于形成具有特定位置Ni和Mn的有序钛铁矿型结构的困难,这可能是由于合成过程中形成的反位缺陷的形成而导致的,这最终会影响MnNiO 3的物理性能。
更新日期:2017-11-07
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