论文标题

二维(2D)Gase的第一原理量子蒙特卡洛研究

A first-principles Quantum Monte Carlo study of two-dimensional (2D) GaSe

论文作者

Wines, Daniel, Saritas, Kayahan, Ataca, Can

论文摘要

二维(2D)过渡后金属硫化剂(PTMC)由于其合适的带隙和较低的激子结合能引起了人们的关注,这使得它们更适合于电子,光学和水的拆分设备,而不是石墨烯和单层过渡器过渡金属二甲化合物(TMDS)。在预测的2D PTMC中,GASE已被可靠地合成并实验表征。尽管这一事实,诸如晶格参数和频带特征之类的数量取决于使用了哪种密度功能理论(DFT)功能。尽管多体扰动理论(GW近似)已用于纠正电子结构并获得2D GASE的激发态性能,并使用求解伯特 - 钙板方程(BSE)来找到光间隙,但我们发现结果很大程度上取决于起始波函数。为了纠正这些差异,我们采用了多体扩散蒙特卡洛(DMC)方法来计算GASE的地面和激发态特性,因为DMC对试验波函数的依赖性较弱。我们使用可用的实验数据,DFT [局部密度近似,Perdew-Burke-ernzerhof(PBE),强烈约束且适当的范围(SCAN)元GGGA和混合(HSE06)功能]和GW-BSE(使用PBE和Scan波波函数)进行基准测试。我们的发现证实单层GASE是一种间接间隙半导体(伽马米),具有与实验和低激子结合能密切一致的准粒子电子间隙。我们还使用DMC和各种DFT方法对最佳晶格参数,粘性能量和基态电荷密度进行基准测试。我们的目标是为原始单层GASE提供终端理论基准,该基准将在使用DMC方法的2D PTMC中进一步研究。

Two-dimensional (2D) post-transition metal chalcogenides (PTMC) have attracted attention due to their suitable band gaps and lower exciton binding energies, making them more appropriate for electronic, optical and water-splitting devices than graphene and monolayer transition metal dichalcogenides (TMDs). Of the predicted 2D PTMCs, GaSe has been reliably synthesized and experimentally characterized. Despite this fact, quantities such as lattice parameters and band character vary significantly depending on which density functional theory (DFT) functional is used. Although many-body perturbation theory (GW approximation) has been used to correct the electronic structure and obtain the excited state properties of 2D GaSe, and solving the Bethe-Salpeter equation (BSE) has been used to find the optical gap, we find that the results depend strongly on the starting wavefunction. In attempt to correct these discrepancies, we employed the many-body Diffusion Monte Carlo (DMC) method to calculate the ground and excited state properties of GaSe because DMC has a weaker dependence on the trial wavefunction. We benchmark these results with available experimental data, DFT [local-density approximation, Perdew-Burke-Ernzerhof (PBE), strongly constrained and appropriately normed (SCAN) meta-GGA, and hybrid (HSE06) functionals] and GW-BSE (using PBE and SCAN wavefunctions) results. Our findings confirm monolayer GaSe is an indirect gap semiconductor (Gamma-M) with a quasiparticle electronic gap in close agreement with experiment and low exciton binding energy. We also benchmark the optimal lattice parameter, cohesive energy and ground state charge density with DMC and various DFT methods. We aim to present a terminal theoretical benchmark for pristine monolayer GaSe, which will aide in the further study of 2D PTMCs using DMC methods.

扫码加入交流群

加入微信交流群

微信交流群二维码

扫码加入学术交流群,获取更多资源