Third-Order Optical Nonlinearity in Two-Dimensional Transition Metal Dichalcogenides

We present a detailed calculation of the linear and nonlinear optical response of four types of monolayer twodimensional (2D) transition-metal dichalcogenides (TMDCs), having the formula MX₂ with M=Mo, W and X=S, Se. The calculations are based on 6-band tight-binding model of TMDCs, and then performing a semi-classical perturbation analysis of response functions. We numerically calculate the linear χ_μν⁽¹⁾ (-ω;ω) and nonlinear surface susceptibility tensors χ_μνζη⁽³⁾(-ω_Σ; ω_r; ω_s; ω_t) with ω_Σ=ω_r+ω_s+ω_t. Both non-degenerate and degenerate cases are studied for thirdharmonic generation and nonlinear refractive index, respectively. Computational results obtained with no external fitting parameters are discussed regarding two recent reported experiments on MoS₂, and thus we can confirm the extraordinarily strong optical nonlinearity of TMDCs. As a possible application, we demonstrate generation of a π/4-rotated squeezed state by means of nonlinear response of TMDCs, in a silica micro-disk resonator covered with the 2D material. Our proposed method will enable accurate calculations of nonlinear optical response, such as four-wave mixing and highharmonic generation in 2D materials and their heterostructures, thus enabling study of novel functionalities of 2D photonic integrated circuits.     

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.     

Interlayer coupling effect in van der Waals heterostructures of transition metal dichalcogenides

Van der Waals(vdW)heterobilayers formed by two-dimensional(2D)transition metal dichalcogenides(TMDCs)created a promising platform for various electronic and optical properties,ab initio band results indicate that the band offset of type-Ⅱband alignment in TMDCs vdW heterobilayer could be tuned by introducing Janus WSSe monolayer,instead of an external electric field.On the basis of symmetry analysis,the allowed interlayer hopping channels of TMDCs vdW heterobilayer were determined,and a four-level k·p model was developed to obtain the interlayer hopping.Results indicate that the interlayer coupling strength could be tuned by interlayer electric polarization featured by various band offsets.Moreover,the difference in the formation mechanism of interlayer valley excitons in different TMDCs vdW heterobilayers with various interlayer hopping strength was also clarified.     

范德华力对双壁碳纳米管轴向压缩屈曲行为的影响

使用分子动力学方法研究几种不同半径尺寸的单壁碳纳米管组成的双壁碳管，预测了其初始稳定构型；分析了其自由弛豫阶段的特征；并模拟了它们在轴向压缩载荷作用下的屈曲行为；研究了不同层间距导致的范德华力变化对屈曲行为的影响.采用Tersoff-Brenner势描述单壁碳纳米管内原子间作用，Lennard-Jones势描述内外层间的范德华相互作用.计算结果表明：在通常意义下的双壁管间距(约0.34 nm)外还可以存在稳定的双壁碳管构型，并且这些新的稳定构型表现出了不同的力学性质. 关键词： 双壁碳纳米管 分子动力学 屈曲     

Spin–phonon coupling in van der Waals antiferromagnet VOCl

We report magnetization and Raman spectroscopy study on single crystals of VOCl, a van der Waals antiferromagnetic material. Magnetization measurement confirms an antiferromagnetic transition at 79 K and a magnetic easy axis along crystallographic a direction. The temperature-dependent Raman spectrum reveals five peaks at 30 K. Below the Neel temperature TN, the Raman-active modes 247 cm~(-1) and 404 cm~(-1) remarkably deviate from the standard Boltzmann function,which is ascribed to the strong magnetoelastic coupling between spins and phonons. We further observe an anomaly in 383 cm~(-1) mode at around 150 K. This coincides with the broad maximum in VOCl's magnetic susceptibility, suggesting a development of short-ranged magnetic order at this temperature.     

Electrostatic Potential Anomaly in 2D Janus Transition Metal Dichalcogenides

Symmetry breaking induced exotic physical properties is an eternal topic in scientific community. Due to lack of mirror symmetry, 2D Janus transition metal dichalcogenides (TMDs) exhibit many bizarre features; however, the physical mechanisms of most of these intrinsic properties are still unclear. Herein, a generalized and effective approach is developed to disclose the physical mechanism of electrostatic potential anomaly in 2D Janus TMDs, based on fast Fourier transform and Moore–Penrose generalized inverse matrix for separating Hartree potential and ionic potential from electrostatic potential, and conversely, calculating charge density distribution through Hartree potential. Through extensive numerical simulations and theoretical analyses, the electrostatic potential anomaly is expounded successfully, which is a pending issue in 2D Janus TMDs: the electrostatic potential energy at Se atomic layer is larger than that at S and Te atomic layers, which breaks the periodic law. Such an anomaly could be attributed to the competition between Hartree potential energy and ionic potential energy that emerges as a result of asymmetric charge transfer, atomic layer distance, and atomic species. This approach possesses universality, and is proved to be a robust method in dealing with the issues related to electrostatic potential.     

On the macroscopic theory of temperature-dependent van der Waals forces

We give a simple derivation of the van der Waals free energy of interaction between two semiinfinite media, including effects of nonzero temperature and retardation. The method, an extension of one used by van Kampen and co-workers at the short-distance and low-temperature limits, considers the free energy of electromagnetic surface modes in the region between the two media. The result is the same as derived by Lifshitz and co-workers using Green's function techniques.     

Tunable electronic and optical properties of GaS/GaSe van der Waals heterostructure

We have used first-principles calculations to investigate the electronic and optical properties of GaS/GaSe van der Waals heterostructures formed by stacking two-dimensional GaSe and GaSe monolayers. Our findings confirm that the GaS/GaSe heterostructures transform from an indirect to a direct band gap material for the two stackings considered in this study. In addition, we found that the direct band gaps are 1.780 eV and 1.736 eV for AA and AB stacking, respectively. It is observed that the behavior of the optical properties of AA stacking is similar to AB stacking with some differences in details and both heterostructures located in UV range. The refractive index values are 2.21 (AA pattern) and 2.18 (AB pattern) at zero photon energy limit and increase to 2.937 for AA and 2.18 AB patterns and both located in the visible region. More importantly, the GaS/GaSe heterostructures have a variety of extraordinary electronic and optical properties. Accordingly, these heterostructures can be useful for the solar cell, nanoelectronics, and optoelectronic applications.     

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.     

Lattice Boltzmann Simulation of van der Waals Phase Transition with Chemical Potential

In this paper phase transition of van der Waals gas is simulated by the Boltzmann lattice method. Thermodynamics and chemical potentials have been taken into account.     

Effect of defects on the electronic structure of a PbI2/MoS2 van der Waals heterostructure: A first-principles study

PbI2/MoS2,as a typical van der Waals(vdW)heterostructure,has attracted intensive attention owing to its remarkable electronic and optoelectronic properties.In this work,the effect of defects on the electronic structures of a PbI2/MoS2 heterointerface has been systematically investigated.The manner in which the defects modulate the band structure of PbI2/MoS2,including the band gap,band edge,band alignment,and defect energy-level density within the band gap is discussed herein.It is shown that sulfur defects tune the band gaps,iodine defects shift the positions of the band edge and Fermi level,and lead defects realize the conversions between the straddling-gap band alignment and valence-band-aligned gap,thus enhancing the light-absorption ability of the material.     

Prospects and Opportunities of 2D van der Waals Magnetic Systems

The existence of spontaneous magnetization in low dimensional magnetic systems has attracted intensive studies since the early 60s and research remains very active even now. Only recently, magnetic van der Waals (vdW) systems down to a few layers have been broadly discussed for their magnetic order ground states at finite temperature. The naturally inherited layered structure of the vdW magnetic systems possessing onsite magnetic anisotropy from band electrons can suppress the long-range fluctuations. This provides an excellent vehicle to study the transition of magnetism to 2D limits both theoretically and experimentally. Here the current status of 2D vdW magnetic system and its potential applications are briefly summarized and discussed.     

范德瓦尔斯磁性材料CrOCl变磁性相变的磁力显微镜研究

近年来,二维范德瓦尔斯磁性材料因为在自旋电子学的应用前景而吸引了广泛的关注.CrOCl是一种范德瓦尔斯磁性材料,理论预言其单层具有高达160 K的居里温度,因此吸引了广泛的关注。为了更好的理解这一材料的磁性,我们利用磁力显微镜研究了CrOCl变磁性相变中磁畴结构随磁场的变化。实验发现,在2K下CrOCl样品表面出现随磁场变化的方格条纹,给出了变磁性相比中反铁磁相和铁磁相竞争的图样,并通过二维快速傅里叶变换证实了CrOCl磁性的各向异性。我们的结果为后续研究CrOCl薄层的磁性提供了参考依据。     

Spin orbit torques in Pt-based heterostructures with van der Waals interface

Spin orbit torques(SOTs) in ferromagnet/heavy-metal heterostructures have provided great opportunities for efficient manipulation of spintronic devices. However, deterministically field-free switching of perpendicular magnetization with SOTs is forbidden because of the global two-fold rotational symmetry in conventional heavy-metal such as Pt. Here,we engineer the interface of Pt/Ni heterostructures by inserting a monolayer MoTe_2 with low crystal symmetry. It is demonstrated that the spin orbit efficiency, as well as the out-of-plane magnetic anisotropy and the Gilbert damping of Ni are enhanced, due to the effect of orbital hybridization and the increased spin scatting at the interface induced by MoTe_2.Particularly, an out-of-plane damping-like torque is observed when the current is applied perpendicular to the mirror plane of the MoTe_2 crystal, which is attributed to the interfacial inversion symmetry breaking of the system. Our work provides an effective route for engineering the SOT in Pt-based heterostructures, and offers potential opportunities for van der Waals interfaces in spintronic devices.     

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.     

Review of Raman spectroscopy of two-dimensional magnetic van der Waals materials

Ultrathin van der Waals (vdW) magnets provide a possibility to access magnetic ordering in the two-dimensional (2D) limit, which are expected to be applied in the spintronic devices. Raman spectroscopy is a powerful characterization method to investigate the spin-related properties in 2D vdW magnets, including magnon and spin-lattice interaction, which are hardly accessible by other optical methods. In this paper, the recent progress of various magnetic properties in 2D vdW magnets studied by Raman spectroscopy is reviewed, including the magnetic transition, spin-wave, spin-lattice interaction, symmetry tuning induced by spin ordering, and nonreciprocal magneto-phonon Raman scattering.     

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.     

Structure of van der Waals bound hybrids of organic semiconductors and transition metal dichalcogenides: the case of acene films on MoS2

Transition metal dichalcogenides (TMDC) are important representatives in the emerging field of two‐dimensional materials. At present their combination with molecular films is discussed as it enables the realization of van der Waals bound organic/inorganic hybrids which are of interest in future device architectures. Here, we discuss the potential use of molybdenum disulfide (MoS₂) as supporting substrate for the growth of well‐defined, crystalline organic adlayers. By this means, hybrid systems between the TMDC surface and organic compounds can be prepared, allowing for the profound investigation of mutual optical and electronic coupling mechanisms. As model system, we choose pentacene and perfluoropentacene as prototypical organic semiconductors and analyze their film formation on MoS₂(001) surfaces. In both cases, we observe smooth, crystalline film growth in lying molecular configuration, hence enabling the preparation of well‐defined hybrid systems. By contrast, on defective MoS₂ surfaces both materials adopt an upright molecular orientation and exhibit distinctly different film morphologies. This emphasizes the importance of highly ordered TMDC surfaces with low defect density for the fabrication of well‐defined hybrid systems.     

Large magnetocaloric effect in van der Waals crystal CrBr3

We study the magnetocaloric effect (MCE) in van der Waals (vdW) crystal CrBr₃. Bulk CrBr₃ exhibits a second-order paramagnetic-ferromagnetic phase transition with T_C = 33 K. The maximum magnetic entropy change −ΔS_M near T_C is about 7.2 J·kg⁻¹·K⁻¹ with the maximum adiabatic temperature change ΔT^max_ad = 2.37 K and the relative cooling power RCP= 191.5 J·kg⁻¹ at μ₀H = 5 T, all of which are remarkably larger than those in CrI₃. These results suggest that the vdW crystal CrBr₃ is a promising candidate for the low-dimensional magnetic refrigeration in low temperature region.