扶手椅型缺陷硫化钼纳米带电子性质的第一性原理计算

基于密度泛函理论的第一性原理计算,研究了含空位缺陷的扶手椅型二硫化钼纳米带的电子性质.发现缺陷会导致纳米带结构稳定性降低,单空位钼缺陷和三空位缺陷使得纳米带从半导体变成金属性,而单空位硫缺陷和两种双空位缺陷仅减小纳米带的带隙;电子态密度和能带的本征态表明缺陷纳米带费米能级附近的杂质态主要是缺陷态的贡献.研究了四类半导体性质的纳米带带隙与宽度的关系,对于完整的纳米带,带隙随宽度以3为周期振荡变化;而引入空位缺陷后,纳米带的带隙振荡不再具有周期且振荡幅度变小.同时发现,当缺陷的浓度变小后,缺陷仅使纳米带的带隙减小,不会使其变为金属性.这些结果有望打开其在新型纳电子器件中的应用潜能.     

利用表面修饰调制GaAs纳米线的电子结构

采用第一性原理的密度泛函方法,研究了利用表面修饰来调制GaAs纳米线的电子结构.在计算中考虑了几种不同的表面钝化材料(H、F、Cl、Br和I)对GaAs纳米线电子结构的影响.计算结果表明,不同的原子修饰GaAs纳米线时对其能带结构的调制主要取决于它们对纳米线表面态的饱和能力.表面修饰不仅可以调节GaAs纳米线的能隙大小,而且也可以调制其能隙类型.GaAs纳米线的电子结构由表面效应和量子限制效应共同来决定.使用不同材料修饰表面的GaAs纳米线的能隙随直径的变化幅度并不相同.表面修饰为实现同种直径和同种结构的GaAs纳米线的能带工程提供了一种新的途径.     

利用表面修饰调制GaAs纳米线的电子结构

采用第一性原理的密度泛函方法,研究了利用表面修饰来调制GaAs纳米线的电子结构. 在计算中考虑了几种不同的表面钝化材料（H、F、Cl、Br 和I）对GaAs纳米线电子结构的影响. 计算结果表明,不同的原子修饰GaAs 纳米线时对其能带结构的调制主要取决于它们对纳米线表面态的饱和能力. 表面修饰不仅可以调节GaAs纳米线的能隙大小,而且也可以调制其能隙类型. GaAs纳米线的电子结构由表面效应和量子限制效应共同来决定. 使用不同材料修饰表面的GaAs纳米线的能隙随直径的变化幅度并不相同. 表面修饰为实现同种直径和同种结构的GaAs纳米线的能带工程提供了一种新的途径.     

Li掺杂ZnO的电子结构与电性能的研究

采用密度泛函理论平面波超软赝势方法研究了p型Li掺杂的纤锌矿结构ZnO的能带结构、态密度和电荷分布,并分析了Li掺杂ZnO的电输运性能.结果表明,Li掺杂ZnO具有1.6eV的直接带隙,且为p型半导体,体系费米能级附近的态密度大大提高,在导带和价带中都出现了由Li电子能级形成的能带,其费米能级附近的能带主要由Li的s态、Zn的p态、Zn的d态和O的p态电子构成,且他们之间存在着强相互作用.电输运参数和电输运性能分析结果表明,Li掺杂的ZnO氧化物价带和导带中的载流子有效质量均较大;其载流子输运主要由Li的s态、Zn的p态和O的p态电子完成;Li掺杂有望改善ZnO的电输运性能.     

B、N原子掺杂超长扶手椅型碳纳米管的GTOs-PBC方法研究

使用密度泛函B3LYP/3-21G*方法,并用周期边界条件模型,计算了B、N掺杂纳米管的结构参数、掺杂能量、能带结构和能隙.研究表明,碳纳米管掺杂B、N原子后,能隙均增大,变为半导体.B原子掺杂的碳纳米管具有直接带隙,而N原子掺杂则具有间接带隙,B掺杂的(6,6)和(9,9)管以及N掺杂的(6,6)和(9,9)管的能隙...     

重费米子化合物LiV2 O4电子结构的第一性原理研究

用第一性原理的FP-LMTO能带计算方法研究了重费米子化合物LiV2O4的电子结构.结果表明:费米面附近的导带是由V原子的3d电子形成的宽度为2.5eV的窄能带,是3d态在立方晶体场中具有t2g对称性的子带;它与O的2p轨道构成的能带有近1.9eV的能隙.计算得出的费米能处电子态密度和线性电子比热系数分别是11.1 states/eV f.u.和26.7 mJ/molK2.费米面处的能带色散具有电子型和空穴型两种,呈现出一种复杂的费米面结构.LSDA以及LDA+GGA计算表明, LiV2O4有一个磁矩为每个钒原子1.13μB,总能比LDA基态低约148 meV/f.u.的铁磁性基态.由目前的能带结构计算的结果无法确定这一类Kondo体系的局域磁矩的来源,表明这一化合物中的重费米子行为可能有别于在含有4f和5f稀土的重费米子合金中观察到的局域磁矩与传导电子的交换作用机制,其中存在量子相变的可能.     

g-C_3N_4纳米带的电子结构及光学性质的第一性原理计算（英文）

采用密度泛函理论的第一性原理方法研究了扶手椅型g-C_3N_4纳米带(AC-g-C_3N_4NRs)和锯齿型g-C_3N_4纳米带(ZZ-g-C_3N_4NRs)的电子结构和光学性质。结果表明:AC-g-C_3N_4NRs和ZZ-g-C_3N_4NRs的边缘H原子均能稳定存在。AC-g-C_3N_4NRs的价带顶主要由多数N原子贡献,而ZZ-g-C_3N_4NRs的价带顶主要由CH边缘附近的N原子贡献。AC-g-C_3N_4NRs的导带底主要属于纳米带一侧边缘或两侧边缘附近的C原子和N原子,而ZZ-g-C_3N_4NRs导带底主要属于ZZ-g-C_3N_4NRs的NH边缘附近的C原子和N原子。AC-g-C_3N_4NRs和ZZ-g-C_3N_4NRs的吸收系数和反射率都随纳米带宽度的增加而增加。随着AC-g-C_3N_4NR宽度的增加,吸收系数在低能区域产生明显的蓝移现象。     

SnO2(110)弛豫表面构型与电子结构的第一性原理研究

采用基于第一性原理的密度泛函方法对SnO₂(110)表面的构型和电子结构进行了系统研究. 结果表明, 与理想表面相比, 表面弛豫导致表层五配位Sn原子向体相方向位移, 六配位Sn原子以及表面氧原子往真空方向移动, 而桥氧原子位置基本保持不变. 当表面厚度小于3 nm时, 表面能和表层原子的弛豫大小随着层数的增加出现振荡现象. 由能带计算结果得知, 以桥氧的2p_y/2i>p_z轨道为主要成分的能带出现在体相的带隙中. 进一步考察了弛豫对表面电子结构的影响.     

带隙问题:第一性原理电子能带理论研究现状

电子能带结构是材料最基本的性质之一,对于材料的实际应用具有深刻影响。电子能带结构的理论描述一直以来都是第一性原理理论方法中最具挑战性的问题之一。作为材料理论计算“标准模型”的密度泛函理论,在局域密度近似或广义梯度近似下,存在着著名的“带隙问题”:半导体材料的理论带隙与实验值相比存在着显著的系统性误差。近年来,以改进对带隙的描述为主要目标之一,密度泛函理论领域有很多重要发展。同时,对于带隙问题,与密度泛函理论紧密相关但又有本质区别的另外一类理论方法是基于格林函数的第一性原理多体微扰理论,其中最为流行的GW方法是当前描述材料的电子能带结构最为准确的第一性原理方法,但一直以来都受限于计算量太大而无法应用于更复杂的体系。本文综述了密度泛函理论和格林函数多体理论在电子能带结构问题上的基本原理、最新进展以及存在的挑战性问题。希望通过比较两种理论框架的异同,为未来可能的发展思路提供启发。     

黄铜矿型半导体材料CuAlX2 (X=S,Se, Te)的电子结构和光学性质

采用基于赝势平面波基组的密度泛函理论方法,研究具有黄铜矿结构的CuAlX2(X=S,Se,Te)晶体的电子结构,并预测了它们的线性和非线性光学性质.结果表明:这些化合物具有相似的能带结构,带隙随X原子从S→Se→Te依次减小.三种晶体的静态介电常数、静态折射率和静态倍频系数d36的变化情况与带隙的变化相反,随着X原子自S→Se→Te改变依次递增,但静态双折射率依次递减.该系列化合物的倍频效应主要来源于价带顶附近的占据能带向以Al和X原子的p电子态为主要成分的空带之间的跃迁.在三种晶体中,CuAlTe2除静态双折射率偏小外,其它光学性能要优于CuAlS2和CuAlSe2.     

Electronic and Optical Properties of O-Terminated Armchair Graphene Nanoribbons

The structure, electromagnetic and optical properties of the O-terminated graphene nanorib-bons with armchair edge are studied using first-principles theory. The results show that the O-terminated armchair edge are more stable than the H-terminated ribbons and show metal-lic character. Spin-polarized calculations reveal that the antiferromagnetic state are more stable than the ferromagnetic state. The energy band and density of states analyses show that the O-terminated armchair edge are antiferromagnetic semiconductors. Because of the terminated O atoms, the dielectric function has an evident red shift and the first peak is the strongest with its main contribution derived from the highest valence band. The peaks of the dielectric function, re ection, absorption, energy loss are related to the transition of electrons. Our results suggest that the O-terminated graphene nanoribbons have potential applications in nanoelectronics, opto-electric devices.     

Half metallicity and electronic structures in armchair BCN-hybrid nanoribbons

We study magnetism and electronic structures of armchair BCN-hybrid nanoribbons from density functional theory. Different from armchair graphene nanoribbons, armchair BCN-hybrid nanoribbons are found to present magnetism along the edges of the nanoribbons if B and N atoms are unpaired in the nanoribbons. Intriguing spin-polarized bands, including magnetic semiconductors, half metals, and magnetic metals, are obtained in the armchair nanoribbons with both the edges composed of C and N atoms. The spin polarization in these armchair nanoribbons is ascribed to the appearance of the unsaturated electronic states in the systems. The magnetic metallicity can be tuned further to half metallicity by adsorbing O atoms at appropriate positions in the ribbons. The electronic structures of the nanoribbons without spin polarization are also analyzed. Our studies provide understanding of the magnetism mechanisms and the electronic properties and most importantly, how to achieve half metallicity in low-dimensional BCN-hybrid systems.     

Quenching of local magnetic moment in oxygen adsorbed graphene nanoribbons

The electronic and magnetic properties of oxidized zigzag and armchair graphene nanoribbons, with hydrogen passivated edges, have been investigated from ab initio pseudopotential calculations within the density functional scheme. The oxygen molecule in its triplet state is adsorbed most stably at the edge of a zigzag nanoribbon. The Stoner metallic behavior of the ferromagnetic nanoribbons and the Slater insulating (ground state) behavior of the antiferromagnetic nanoribbons remain intact upon oxygen adsorption. The formation of a spin-paired C-O bond drastically reduces the local atomic magnetic moment of carbon at the edge of the ferromagnetic zigzag ribbon.     

Magnetic and electronic properties of α-graphyne nanoribbons

Based on the first-principles calculations, we investigate the magnetic and electronic properties of α-graphyne nanoribbons (NRs). We show that all the armchair α-graphyne NRs are nonmagnetic semiconductors with band gaps as a function of ribbon widths. The zigzag α-graphyne NRs are found to have magnetic semiconducting ground state with ferromagnetic ordering at each edge and opposite spin orientation between the two edges. Under the application of transverse electric field, we further predict the existence of half-metallicity in the zigzag NRs which strongly depends on the width of the ribbon.     

Role of Edge Geometry and Magnetic Interaction in Opening Bandgap of Low‐Dimensional Graphene

By using a size‐dependent cohesive energy formula for two‐dimensional coordination materials, the bandgap openings of ideal graphene quantum dots (GQDs) and nanoribbons (GNRs) have been investigated systematically regarding dimension, edge geometry, and magnetic interaction. Results demonstrate that the bandgap openings in GQDs can be dominated by the change of atomic cohesive energy. Relative to zigzag GQDs, the openings in the armchair ones are more substantial, attributed to its edge instability. The change of cohesive energy can also lead to bandgap openings in zigzag and armchair GNRs. The contribution from the interedge magnetic interaction in zigzag GNRs is negligible, while the cohesive‐energy induced openings in armchair GNRs can oscillate according to the so‐called full‐wavelength effect, depending on the width. The model prediction provides physicochemical insight into the bandgap openings in graphene.     

The study of electronic and optical properties of ZnO/MoS2 and its vacancy heterostructures by first principles

Based on the first principles calculation, the effects of vacancies on the structural, electronic and optical properties of ZnO/MoS₂ heterostructure are investigated in this work. The results show that vacancies could exist stably in the heterojunctions and cause a significant decrease in bandgap. ZnO/MoS₂ with an O vacancy maintains semiconductor property with a bandgap of 0.119 eV, while heterostructure with a Zn vacancy exhibits metallic characteristic. Furthermore, the absorption capability of defective heterojunctions has been extended to infrared light region with obvious redshift. To sum up, vacancy engineering effectively changes the electronic and optical properties of ZnO/MoS₂ heterostructure, which provides a feasible approach for adjusting the optoelectronic properties of two-dimensional heterostructures and broadening their application in functional nanoelectronic and optoelectronic devices.     

Electronic Properties of Triangle Molybdenum Disulfide (MoS2) Clusters with Different Sizes and Edges

The electronic structures and transition properties of three types of triangle MoS₂ clusters, A (Mo edge passivated with two S atoms), B (Mo edge passivated with one S atom), and C (S edge) have been explored using quantum chemistry methods. The highest occupied molecular orbital (HOMO)–lowest unoccupied molecular orbital (LUMO) gap of B and C is larger than that of A, due to the absence of the dangling of edge S atoms. The frontier orbitals (FMOs) of A can be divided into two categories, edge states from S_3p at the edge and hybrid states of Mo_4d and S_3p covering the whole cluster. Due to edge/corner states appearing in the FMOs of triangle MoS₂ clusters, their absorption spectra show unique characteristics along with the edge structure and size.     

Tuning the Properties of Tetracene-Based Nanoribbons by Fluorination and N-Doping

The structural stabilities and electronic properties are studied for the recently synthesized one-dimensional (1-D) tetracene-based nanoribbons with four-membered rings by using first-principles calculation. All three configurations (named as straight, zigzag, and armchair) are stable and exhibit an indirect band gap of 1.46, 0.73, and 0.32 eV, respectively. The band gaps can be effectively tuned by substituting hydrogen with fluorine atoms and by doping with nitrogen atoms. Substituting hydrogen with fluorine atoms leads to gradual decrease of the electronic band gaps of all configurations. Nitrogen doping changes the band gap from indirect to direct, displaying flexibility of tuning the band structure.     

Electronic and magnetic properties of armchair and zigzag graphene nanoribbons

The electronic properties, band gap, and ionization potential of zigzag and armchair graphene nanoribbons are calculated as a function of the number of carbon atoms in the ribbon employing density functional theory at the B3LYP6-31G* level. In armchair ribbons, the ionization potential and band gap show a gradual decrease with length. For zigzag ribbons, the dependence of the band gap and ionization potential on ribbon length is different depending on whether the ribbon has an unpaired electron or not. It is also found that boron and nitrogen zigzag and armchair doped graphene nanoribbons have a triplet ground state and could be ferromagnetic.