Modeling WO3 beyond the Harmonic Approximation: Theoretical Characterization and Thermal Expansion

IF 3.3 3区 化学 Q2 CHEMISTRY, PHYSICAL
Felix Bernhardt, Simone Sanna
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引用次数: 0

Abstract

The structural, thermal, electronic, and optical properties of different WO3 polymorphs are calculated from first principles. Based on density functional theory and the quasi-harmonic approximation, the thermal expansion coefficient and the specific heat capacity as a function of temperature are modeled. Similar trends are observed for all phases, with only a slight dependence on the crystal symmetry. The dielectric function, refractive index, and absorption coefficient are calculated using an efficient combination of G0W0 and time-dependent density functional perturbation theory in the long-range correction approximation. An excellent agreement to experiment can be observed. Finally, Raman spectra for all phases are calculated and discussed based on their symmetry and phononic eigenmodes. The hypothetic cubic phase often employed in theoretical investigations fails to reproduce the aforementioned properties, limiting its application as a simple model for the real polymorphs.

Abstract Image

超越谐波近似的 WO3 建模:理论特性和热膨胀
从第一性原理计算了不同WO3多晶的结构、热、电子和光学性质。基于密度泛函理论和准调和近似,建立了热膨胀系数和比热容随温度变化的模型。在所有相中都观察到类似的趋势,仅对晶体对称性有轻微的依赖。在远程校正近似中,利用G0W0和时变密度泛函摄动理论的有效组合计算了介电函数、折射率和吸收系数。可以观察到与实验结果非常吻合。最后,根据各相的对称性和声子本征模计算并讨论了各相的拉曼光谱。通常用于理论研究的假设立方相不能再现上述性质,限制了其作为实际多晶的简单模型的应用。
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来源期刊
The Journal of Physical Chemistry C
The Journal of Physical Chemistry C 化学-材料科学:综合
CiteScore
6.50
自引率
8.10%
发文量
2047
审稿时长
1.8 months
期刊介绍: The Journal of Physical Chemistry A/B/C is devoted to reporting new and original experimental and theoretical basic research of interest to physical chemists, biophysical chemists, and chemical physicists.
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