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中国物理学会期刊

La2CF2电子、光学及热力学性质的第一性原理研究

First-Principles Study on Electronic, Optical and Thermodynamic Properties of La2CF2

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  • 二维过渡金属碳氮化物(MXene)因其层状结构及可调光电性质而受到广泛关注,但稀土镧基MXene的光学响应及其电子结构起源仍缺乏系统认识。本文基于密度泛函理论,结合声子谱与从头算分子动力学(AIMD)评估La2CF2单层的结构稳定性,并在HSE06杂化泛函层级计算其电子结构与光学性质,进一步采用形变势理论计算其载流子迁移率。结果表明,La2CF2为六方结构,声子谱无虚频且在300 K下AIMD能量与温度稳定波动,验证其动力学与热力学稳定性。La2CF2呈直接带隙半导体特征,价带顶主要由C/F-p态贡献,导带底主要由La-d态主导,CBM和VBM表现出不同的空间电荷分布特征。基于形变势理论计算表明,La2CF2的载流子输运具有一定的面内各向异性,其声学声子散射限制下的理论迁移率处于102 cm2·V-1·s-1量级。光学计算显示La2CF2在可见—紫外区具有宽谱强吸收。

     

    Two-dimensional transition metal carbides and nitrides (MXenes) have attracted extensive attention due to their layered structure and tunable photophysical properties. However, the optical response and electronic structure origin of rare-earth lanthanide-based MXenes remain poorly understood. Based on density functional theory, combined with phonon spectroscopy and ab initio molecular dynamics (AIMD) to evaluate the structural stability of La2CF2 monolayer, and using HSE06 hybrid functional level calculations to assess its electronic structure and optical properties, and further using the deformation potential theory to calculate its carrier mobility. The results show that La2CF2 has a hexagonal structure, the phonon spectrum has no imaginary frequency and the AIMD energy and temperature fluctuate stably at 300 K, verifying its dynamic and thermodynamic stability. La2CF2 exhibits direct bandgap semiconductor characteristics, the valence band top is mainly contributed by C/F-p states, the conduction band bottom is mainly dominated by La-d states, and the CBM and VBM show different spatial charge distribution characteristics. Based on the deformation potential theory calculation, the carrier transport of La2CF2 has certain in-plane anisotropy, and the theoretical mobility under the limitation of acoustic phonon scattering is at the order of 102 cm2·V-1·s-1. Optical calculations show that La2CF2 has wide-spectrum strong absorption in the visible-ultraviolet region.

     

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