β型锑烯热电输运性质的第一性原理研究

利用第一性原理与半经典玻尔兹曼方程，计算并分析β型锑烯的声子色散、声子群速度、声子弛豫时间、晶格热导率及不同温度下的塞贝克系数、电导率和电子热导率随化学势的变化；结果表明：β型锑烯由于非平面六角结构，三支声学声子在Γ点附近均呈线性变化；声学声子对整个晶格热导率的贡献高达96.68%，而光学声子仅仅占到3.32%；由于较大的声光带隙（a-o gap）导致LA支在声子群速度和弛豫时间中占据主导地位，从而增大了LA支声子对整个热导的贡献；热电优值随温度的升高而增大，在费米面附近其绝对值最大可达0.275.     

二维Mo2C的晶格热导率的第一性原理研究

Mo2C是构建Mxene基器件的重要材料之一,对Mo2C二维材料声子输运的理解非常必要。文章结合第一性原理方法和声子玻尔兹曼输运方程,研究了二维Mo2C材料的晶格热导率。研究表明,室温下二维Mo2C导热系数非常低,其锯齿方向和扶手椅方向的晶格热导率分别为7.20 和 5.04 W/mK。计算了声学振动和光学振动模式对晶格热导率的贡献,揭示总热导率主要由面内声学横波的振动模式所贡献。还进一步计算了声子群速度、声子弛豫时间、三声子散射空间和模式格林艾森参数,发现二维Mo2C中的声子群速度和声子弛豫时间对晶格传输有重要的影响。     

二维MoS2/MoSe2异质材料的电子结构和热电性质研究

利用密度泛函理论结合玻尔兹曼输运理论计算体相和双层二维MoS₂/MoSe₂异质材料的热电性质. 计算表明,体相MoS₂/MoSe₂异质材料的热电性质比之于MoSe₂会有较大程度的提高. 该异质材料热电性质的提高主要源于异质材料本身带隙的减小以及层间的范德瓦尔斯相互作用. 二维MoS₂/MoSe₂异质材料存在热电应用的可能性.     

Controlled vapor growth of 2D magnetic Cr_2Se_3 and its magnetic proximity effect in heterostructures

Two-dimensional(2 D) magnetic materials have aroused tremendous interest due to the 2 D confinement of magnetism and potential applications in spintronic and valleytronic devices. However, most of the currently 2 D magnetic materials are achieved by the exfoliation from their bulks, of which the thickness and domain size are difficult to control, limiting the practical device applications. Here, we demonstrate the realization of thickness-tunable rhombohedral Cr_2Se_3 nanosheets on different substrates via the chemical vapor deposition route. The magnetic transition temperature at about 75 K is observed. Furthermore, van der Waals heterostructures consisting of Cr_2Se_3 nanosheets and monolayer WS_2 are constructed.We observe the magnetic proximity effect in the heterostructures, which manifests the manipulation of the valley polarization in monolayer WS_2. Our work contributes to the vapor growth and applications of 2 D magnetic materials.     

Tuning electronic properties of the S_2/graphene heterojunction by strains from density functional theory

Based on the density functional calculations, the structural and electronic properties of the WS_2/graphene heterojunction under different strains are investigated. The calculated results show that unlike the free mono-layer WS_2, the monolayer WS_2 in the equilibrium WS_2/graphene heterojunctionis characterized by indirect band gap due to the weak van der Waals interaction. The height of the schottky barrier for the WS_2/graphene heterojunction is 0.13 eV, which is lower than the conventional metal/MoS_2 contact. Moreover, the band properties and height of schottky barrier for WS_2/graphene heterojunction can be tuned by strain. It is found that the height of the schottky barrier can be tuned to be near zero under an in-plane compressive strain, and the band gap of the WS_2 in the heterojunction is turned into a direct band gap from the indirect band gap with the increasing schottky barrier height under an in-plane tensile strain. Our calculation results may provide a potential guidance for designing and fabricating the WS_(2~-)based field effect transistors.     

Anomalous layer thickness dependent thermal conductivity of Td-WTe2 through first-principles calculation

The thickness dependent in-plane thermal conductivity of layered Tungsten ditelluride (WTe₂) is investigated by first-principles calculation. With the layer number increasing from one to infinite, the thermal conductivity displays a decrease to increase trend. The underlying mechanism is attributed to the change of the phonon dispersion relations. As the layer number increases, optical phonon branches shift downward, which provide more channels for the Umklapp scattering, and result in the decrease of the thermal conductivity. Furthering increasing the layer number makes those low-frequency optical phonon branches having high group velocity and leads to the increase of the lattice thermal conductivity.     

How Does van der Waals Confinement Enhance Phonon Transport?

We study the mechanism of van der Waals(vdW)interactions on phonon transport in atomic scale,which would boost developments in heat management and energy conversion.Commonly,the vdW interactions are regarded as a hindrance in phonon transport.Here we propose that the vdW confinement can enhance phonon transport.Through molecular dynamics simulations,it is realized that the vdW confinement is able to make more than two-fold enhancement on thermal conductivity of both polyethylene single chain and graphene nanoribbon.The quantitative analyses of morphology,local vdW potential energy and dynamical properties are carried out to reveal the underlying physical mechanism.It is found that the confined vdW potential barriers reduce the atomic thermal displacement magnitudes,leading to less phonon scattering and facilitating thermal transport.Our study offers a new strategy to modulate the phonon transport.     

尿素夹层二硫化钛化合物的合成及其热、电输运性质研究(英文)

我们成功的制备出了含不同成分尿素的夹层化合物(NH2CONH2)xTiS2,并研究了它们在低温(5～310K)下的热、电输运性质.夹层后晶格常数、热、电输运行为的变化也证实了尿素分子成功的夹层到TiS2的范德华尔斯层间.研究结果表明:尿素分子的夹层成功的降低了材料的热导率,特别是在浓度为12.5mmol/L尿素的苯溶液中合成的样品的热导率大约1.5Wm-1 K-1(仅为纯TiS2的50%),而且尿素分子的夹层使得材料在低温下的导电行为从金属性转变为半导体性.     

Thermally induced band hybridization in bilayer-bilayer MoS_2/WS_2 heterostructure

Transition metal dichalcogenides(TMDs), being valley selectively, are an ideal system hosting excitons. Stacking TMDs together to form heterostructure offers an exciting platform to engineer new optical and electronic properties in solid-state systems. However, due to the limited accuracy and repetitiveness of sample preparation, the effects of interlayer coupling on the electronic and excitonic properties have not been systematically investigated. In this report, we study the photoluminescence spectra of bilayer-bilayer MoS_2/WS_2 heterostructure with a type Ⅱ band alignment. We demonstrate that thermal annealing can increase interlayer coupling in the van der Waals heterostructures, and after thermally induced band hybridization such heterostructure behaves more like an artificial new solid, rather than just the combination of two individual TMD components. We also carry out experimental and theoretical studies of the electric controllable direct and indirect infrared interlayer excitons in such system. Our study reveals the impact of interlayer coupling on interlayer excitons and will shed light on the understanding and engineering of layer-controlled spin-valley configuration in twisted van der Waals heterostructures.     

Tuning band alignment and optical properties of 2D van der Waals heterostructure via ferroelectric polarization switching

Favourable band alignment and excellent visible light response are vital for photochemical water splitting. In this work, we have theoretically investigated how ferroelectric polarization and its reversibility in direction can be utilized to modulate the band alignment and optical absorption properties. For this objective, 2D van der Waals heterostructures (HTSs) are constructed by interfacing monolayer MoS₂ with ferroelectric In2Se3. We find the switch of polarization direction has dramatically changed the band alignment, thus facilitating different type of reactions. In In₂Se₃/MoS₂/In₂Se₃ heterostructures, one polarization direction supports hydrogen evolution reaction and another polarization direction can favour oxygen evolution reaction. These can be used to create tuneable photocatalyst materials where water reduction reactions can be selectively controlled by polarization switching. The modulation of band alignment is attributed to the shift of reaction potential caused by spontaneous polarization. Additionally, the formed type-II van der Waals HTSs also significantly improve charge separation and enhance the optical absorption in the visible and infrared regions. Our results pave a way in the design of van der Waals HTSs for water splitting using ferroelectric materials.     

基于AsP/MoS2异质结的偏振光电探测器

线偏振光的探测能力是评价偏振光电探测器件的重要指标。黑砷磷(AsP)是一种较为稳定的平面内各向异性材料,由于其面内结构各向异性,其对线偏振光较为敏感,在偏振探测领域有着重要的应用潜力。本文介绍了一种基于AsP/MoS2的高度偏振敏感光电探测器。由于AsP各向异性的光吸收、MoS2有效的载流子收集和输运能力以及范德华异质结对暗电流的抑制作用,该光电探测器实现了大于300的电流开关比,0.27 A/W的电流光响应度以及2×10^10 Jones的比探测率。更重要的是,此类光电探测器在638 nm波段实现了高达3.06二向色性比的偏振特性。这些实验结果表明AsP/MoS2异质结构在偏振光电探测领域有着广阔的应用前景。     

二维范德瓦尔斯异质结构的制备与物性研究

二维范德瓦尔斯材料(可简称二维材料)已发展成为备受瞩目的材料大家族,而由其衍生的二维范德瓦尔斯异质结构的集成、性能及应用是现今凝聚态物理和材料科学领域的研究热点之一.二维范德瓦尔斯异质结构为探索丰富多彩的物理效应和新奇的物理现象,以及构建新型的自旋电子学器件提供了灵活而广阔的平台.本文从二维材料的转移技术着手,介绍二维范德瓦尔斯异质结构的构筑、性能及应用.首先,依据湿法转移和干法转移的分类,详细介绍二维范德瓦尔斯异质结构的制备技术,内容包括转移技术的通用设备、常用转移方法的具体操作步骤、三维操纵二维材料的方法、异质界面清洁.随后介绍二维范德瓦尔斯异质结构的性能和应用,重点介绍二维磁性范德瓦尔斯异质结构,并列举在二维范德瓦尔斯磁隧道结和摩尔超晶格领域的应用.因此,二维材料转移技术的发展和优化将进一步助力二维范德瓦尔斯异质结构在基础科学研究和实际应用上取得突破性的成果.     

Computational screening of vdWs heterostructures of BSe with MoSe2 and WSe2 as sustainable hydrogen production materials

Recently, fabricating type-II vertical van der Waals (vdWs) heterostructure is a promising material for hydrogen production. The absorption capability, charge density distributions, band alignments and electronic properties of the monolayers and heterostructures are systematically investigated using computational studies. Using ab initio molecular dynamics, binding energy and phonon calculations, the stability of the heterostructures are verified. Both heterostructures are type-II materials, which can increase the separation of charge carriers. Moreover, the charge density difference and the potential drop across the interface of MSe₂/BSe creates a high built-in electric field that can prevent the recombination of charge carriers. We found that the visible-light optical properties of both heterostructures are much enhanced with suitable bandgap energy for water splitting. The band alignment suggests that the heterostructures straddle water redox potentials in acid solutions (0 < pH < 7). Our study predicted that MSe₂/BSe vdW heterostructures have great potential for photocatalytic hydrogen production.     

二维范德瓦尔斯异质结构的制备与物性研究

二维范德瓦尔斯材料(可简称二维材料)已发展成为备受瞩目的材料大家族,而由其衍生的二维范德瓦尔斯异质结构的集成、性能及应用是现今凝聚态物理和材料科学领域的研究热点之一.二维范德瓦尔斯异质结构为探索丰富多彩的物理效应和新奇的物理现象,以及构建新型的自旋电子学器件提供了灵活而广阔的平台.本文从二维材料的转移技术着手,介绍二维范德瓦尔斯异质结构的构筑、性能及应用.首先,依据湿法转移和干法转移的分类,详细介绍二维范德瓦尔斯异质结构的制备技术,内容包括转移技术的通用设备、常用转移方法的具体操作步骤、三维操纵二维材料的方法、异质界面清洁.随后介绍二维范德瓦尔斯异质结构的性能和应用,重点介绍二维磁性范德瓦尔斯异质结构,并列举在二维范德瓦尔斯磁隧道结和摩尔超晶格领域的应用.因此,二维材料转移技术的发展和优化将进一步助力二维范德瓦尔斯异质结构在基础科学研究和实际应用上取得突破性的成果.     

应力调控BlueP/XTe2(X=Mo,W)范德瓦耳斯异质结电子结构及光学性质理论研究

通过第一性原理计算探讨了蓝磷烯与过渡金属硫化物MoTe₂/WTe₂形成范德瓦耳斯异质结的电子结构和光学性质,以及施加双轴应力对相关性质的影响.计算结果表明,形成BlueP/XTe₂(X=Mo,W)异质结,二者能带排列为间接带隙type-Ⅱ并有较强的红外光吸收,同时屏蔽特性增强.随压缩应力增加,BlueP/XTe₂转变为直接带隙type-Ⅱ能带排列最后转变为金属性;随拉伸应力增加,异质结转变为间接带隙type-Ⅰ能带排列.外加应力也能有效调控异质结的光吸收性质,随压缩应力增加吸收边红移,光吸收响应拓展至中红外光谱区且吸收系数增大;BlueP/MoTe₂较BlueP/WTe₂在中红外至红外光区间表现出更强的光吸收响应;静态介电常数ε1(0)大幅增加.结果表明,压缩应力对BlueP/MoTe₂和BlueP/WTe₂能带排列、光吸收特性均有显著的调控作用,其中BlueP/MoTe₂对调控更敏感,这些特性也使BlueP/XTe₂异质结在窄禁带中红外半导体材料及光电器件具有令人期待的应用价值.     

Effect of normal processes on thermal conductivity of germanium,silicon and diamond

The effect of normal scattering processes is considered to redistribute the phonon momentum in (a) the same phonon branch — KK-S model and (b) between different phonon branches — KK-H model. Simplified thermal conductivity relations are used to estimate the thermal conductivity of germanium, silicon and diamond with natural isotopes and highly enriched isotopes. It is observed that the consideration of the normal scattering processes involving different phonon branches gives better results for the temperature dependence of the thermal conductivity of germanium, silicon and diamond with natural and highly enriched isotopes. Also, the estimation of the lattice thermal conductivity of germanium and silicon for these models with the consideration of quadratic form of frequency dependences of phonon wave vector leads to the conclusion that the splitting of longitudinal and transverse phonon modes, as suggested by Holland, is not an essential requirement to explain the entire temperature dependence of lattice thermal conductivity whereas KK-H model gives a better estimation of the thermal conductivity without the splitting of the acoustic phonon modes due to the dispersive nature of the phonon dispersion curves.      

表面共振圆环结构对Si纳米线热传导的调控

利用声子的波动性,在纳米线表面引入共振结构,可以有效阻碍声子输运.为进一步优化共振结构,本文基于平衡态分子动力学(EMD)方法,研究表面共振圆环结构的高度和宽度对Si纳米线热输运性质的影响.结果表明：随着共振圆环高度的增加,Si纳米线的热导率逐渐减小,最大减幅可达61.9%.当高度达到2nm以后,热导率基本不再变化.共振圆环宽度则对热导率的影响较小.声子色散关系中出现的平带,证实了共振圆环引起的声子共振效应;最低共振频率的变化说明了共振圆环中的声子波长决定了共振圆环高度对纳米线热导率的最大影响程度.研究进一步发现,随着共振圆环高度的增加,声学支声子对热导率贡献的比重变小.本文研究结果对高效热电材料和隔热材料的微纳结构设计提供了一种新的思路.     

Artificially controlled synthesis of graphene intramolecular heterojunctions for phonon engineering

Because phonons are the main carriers for graphene heat transfer, modifying the dynamic properties of the crystal lattice by isotopes modulates the phonon behavior and alters the thermal properties. Here we demonstrate an artificially controlled texture synthesis of ¹²C‐graphene/¹³C‐graphene heterostructures via chemical vapor deposition and an O₂ plasma etching. The electrical and thermal properties of the graphene across the heterojunction show that ¹²C‐graphene and ¹³C‐ graphene are electronically connected as resistors in series, while the thermal conductivity across the junction is dramatically reduced due to the suppressed phonon propagation, which causes the conductivity across the junction to be lower than that of graphene sheets with randomly mixed isotopes. These findings should help realize novel two‐dimensional graphene thermoelectric devices where phonon modulation controls the electrons and heat transport independently. (© 2014 WILEY‐VCH Verlag GmbH &Co. KGaA, Weinheim)     

A self-driven photodetector based on a SnS2/WS2 van der Waals heterojunction with an Al2O3 capping layer

Photodetectors based on two-dimensional (2D) materials have attracted considerable attention because of their unique properties. To further improve the performance of self-driven photodetectors based on van der Waals heterojunctions, a conductive band minimum (CBM) matched self-driven SnS₂/WS₂ van der Waals heterojunction photodetector based on a SiO₂/Si substrate has been designed. The device exhibits a positive current at zero voltage under 365 nm laser illumination. This is attributed to the built-in electric field at the interface of the SnS₂ and WS₂ layer, which will separate and transport the photogenerated carriers, even at zero bias voltage. In addition, the Al₂O₃ layer is covered by the surface of the SnS₂/WS₂ photodetector to further improve the performance, because the Al₂O₃ layer will introduce tensile stress on the surface of the 2D materials leading to a higher electron concentration and smaller effective mass of electrons in the films. This work provides an idea for the research of self-driven photodetectors based on a van der Waals heterogeneous junction.     

Electronic Transport and Thermopower in 2D and 3D Heterostructures—A Theory Perspective

The impact of interfaces and heterojuctions on the electronic and thermoelectric transport properties of materials is discussed herein. Recent progress in understanding electronic transport in heterostructures of 2D materials ranging from graphene to transition metal dichalcogenides, their homojunctions (grain boundaries), lateral heterojunctions (such as graphene/MoS₂ lateral interfaces), and vertical van der Waals heterostructures is reviewed. Work on thermopower in 2D heterojunctions, as well as their applications in creating devices such as resonant tunneling diodes (RTDs), is also discussed. Last, the focus turns to work in 3D heterostructures. While transport in 3D heterostructures has been researched for several decades, here recent progress in theory and simulation of quantum effects on transport via the Wigner and non‐equilibrium Green's functions approaches is reviewed. These simulation techniques have been successfully applied toward understanding the impact of heterojunctions on transport properties and thermopower, which finds applications in energy harvesting, and electron resonant tunneling, with applications in RTDs. In conclusion, tremendous progress has been made in both simulation and experiments toward the goal of understanding transport in heterostructures and this progress will soon be parlayed into improved energy converters and quantum nanoelectronic devices.