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中国物理学会期刊

双轴应变对Co掺杂单层MoS2磁学和光学性质影响的理论研究

Effect of biaxial strain on magnetic and optical properties in Co doped monolayer MoS2 studied by the first-principles calculation

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  • 单层MoS2基磁性半导体的实现及其自旋态的调控规律对二维自旋电子器件的开发和利用具有重要的科学价值.本文利用基于密度泛函理论的第一性原理计算方法系统研究了双轴应变对Co掺杂单层MoS2的电子结构、磁学和光学性质的影响.研究表明:不同双轴应变下,Co掺杂的MoS2(CoMo)体系具有不同的电子结构,-9%—-6%应变范围内,CoMo体系产生大小为1.00 μB的局域磁矩,-5%—9%应变范围内,CoMo体系产生大小为3.00 μB的磁矩;磁矩之间的耦合类型随应变呈振荡趋势,3%应变下CoMo体系铁磁(Ferromagnetic,FM)耦合的强度最大,磁耦合机制由d-p-d超交换作用主导;此外,Co的掺杂提升了CoMo体系中价电子的跃迁概率和光生电子空穴对的分离效率,使得掺杂体系的光催化性能得到了很大的改善,同时提升了CoMo体系对可见光区和红外光区光子的吸收幅度,光学吸收谱的吸收边发生了红移,而拉伸应变则进一步提升了CoMo体系在可见光区和红外光区的光学性能.

    It is scientifically significant to realize monolayer MoS2-based magnetic semiconductors and to regulate the spin states of MoS2 for the development and application of two-dimensional (2D) spintronic devices. In this work, we systematically studied the effects of biaxial strain on the electronic structure, magnetic and optical properties of Co doped monolayer MoS2 (CoMo) systems using the first-principles calculations based on density functional theory (DFT). Our results indicate that the electronic structure, magnetic and optical properties of CoMo systems are closely related to biaxial strain. First, strain regulates the energy level sequences of Co-d orbitals. The electronic configurations vary with strains as follows: a+a-e1+e1-e2+e2- for strains between -9% and -6%, a+e1+a-e2+e1-e2- for -5% to -4%, e1+e2+a+a-e1-e2- for -3% to 0%, a+e1+e2+a-e1-e2- for 1% to 6%, and e1+a+a-e1-e2+e2- for 7% to 9%, respectively. Second, strain influences the occupancy of Co-d orbitals, thereby affecting the magnetic properties. In the strain range of -9%—-6%, the CoMo systems exhibit a local magnetic moment of 1.00 μB, and the coupling between such two moments is ferromagnetic (FM). Within the strain range of -5%—9%, the CoMo systems produce a magnetic moment of 3.00 μB, and the coupling between the magnetic moments is antiferromagnetic (AFM) in the range of -5%—-4%, translates to FM states in the range of -3%— 6%, and then changes to AFM states within range of 7%—9%. Among them, the FM coupling strength of the CoMo system is strongest at 3% strain, which is favorable for achieving a high Curie temperature (TC) in MoS2-based magnetic semiconductors. These oscillatory magnetic interactions are attributed to the d-p-d superexchange and d-d direct-exchange mechanisms. Third, tensile strain enhances the optical properties of CoMo systems. Compared to undoped MoS2, the increased complex dielectric function in the low-energy light region enhances the valence electron transition probability and the separation efficiency of photogenerated electron-hole pairs, leading to a significant improvement in photocatalytic performance for the CoMo doped systems. Moreover, the impurity energy levels introduced by Co are located in the band-gap, which reduces the energy for valence electrons to transition to empty bands, thereby increasing photon absorption in the visible and infrared regions in CoMo doped systems. Meanwhile, the absorption edge undergoes a red shift, and tensile strain further improves the optical performance of the Co doped monolayer MoS2 systems in the visible and infrared regions. Finally, dynamic stability analysis under strain reveals that CoMo systems are unstable as strain in the range of -9%—-4%. Combined with the magnetic, optical properties, and structural stability of CoMo systems, the strain should be in the range of 1%—6%. The results presented here provide a novel approach for fabricating MoS2-based magnetic semiconductors with superior optical properties.

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