硅烯的化学功能化

硅烯是一种零能隙的狄拉克费米子材料,对其能带结构的有效调控进而打开带隙是硅烯进一步器件化的基础.而化学功能化是调控二维材料的结构和电子性质的一种有效方法.本文简要介绍了近几年在硅烯的化学功能化方面取得的进展,主要包括硅烯的氢化、氧化、氯化以及其他几种可能的化学修饰方法.     

Growth mechanism and modification of electronic and magnetic properties of silicene

Silicene, a monolayer of silicon atoms arranged in a honeycomb lattice, has been undergoing rapid development in recent years due to its superior electronic properties and its compatibility with mature silicon-based semiconductor technology. The successful synthesis of silicene on several substrates provides a solid foundation for the use of silicene in future microelectronic devices. In this review, we discuss the growth mechanism of silicene on an Ag(111) surface, which is crucial for achieving high quality silicene. Several critical issues related to the electronic properties of silicene are also summarized, including the point defect effect, substrate effect, intercalation of alkali metal, and alloying with transition metals.     

Electronic structure of silicene

In this topical review, we discuss the electronic structure of free-standing silicene by comparing results obtained using different theoretical methods. Silicene is a single atomic layer of silicon similar to graphene. The interest in silicene is the same as for graphene, in being two-dimensional and possessing a Dirac cone. One advantage of silicene is due to its compatibility with current silicon electronics. Both empirical and first-principles techniques have been used to study the electronic properties of silicene. We will provide a brief overview of the parameter space for first-principles calculations.However, since the theory is standard, no extensive discussion will be included. Instead, we will emphasize what empirical methods can provide to such investigations and the current state of these theories. Finally, we will review the properties computed using both types of theories for free-standing silicene, with emphasis on areas where we have contributed.Comparisons to graphene is provided throughout.     

Electronic properties of silicene in BN/silicene van der Waals heterostructures

Silicene is a promising 2D Dirac material as a building block for van der Waals heterostructures(vd WHs). Here we investigate the electronic properties of hexagonal boron nitride/silicene(BN/Si) vd WHs using first-principles calculations.We calculate the energy band structures of BN/Si/BN heterostructures with different rotation angles and find that the electronic properties of silicene are retained and protected robustly by the BN layers. In BN/Si/BN/Si/BN heterostructure, we find that the band structure near the Fermi energy is sensitive to the stacking configurations of the silicene layers due to interlayer coupling. The coupling is reduced by increasing the number of BN layers between the silicene layers and becomes negligible in BN/Si/(BN)_3/Si/BN. In(BN)_n/Si superlattices, the band structure undergoes a conversion from Dirac lines to Dirac points by increasing the number of BN layers between the silicene layers. Calculations of silicene sandwiched by other 2D materials reveal that silicene sandwiched by low-carbon-doped boron nitride or HfO_2 is semiconducting.     

Spin-current pump in silicene

We report a theoretical study of pumped spin currents in a silicene-based pump device, where two time-dependent staggered potentials are introduced through the perpendicular electric fields and a magnetic insulator is considered in between the two pumping potentials to magnetize the Dirac electrons. It is shown that giant spin currents can be generated in the pump device because the pumping can be optimal for each transport mode, the pumping current is quantized. By controlling the relevant parameters of the device, both pure spin currents and fully spin-polarized currents can be obtained.Our results may shed a new light on the generation of pumped spin currents in Dirac-electron systems.     

Chemical modification of chitosan under high-intensity ultrasound

Chitosan (CTS), a biocompatible, biodegradable, non-toxic polymer, dissolves in water only if pH is lowered under 6.5, when a substantial fraction of the amino groups is protonated. Its range of application has been much extended by partially depolymerising it or converting it to water-soluble derivatives. Working under high-intensity ultrasound at 17.8-18.5 kHz, using either a simple horn or a cup horn, we achieved a controlled depolymerization of CTS, also prepared in high yields several derivatives that can be useful intermediates for further chemical modification, as well as several water-soluble derivatives that lend themselves to a host of industrial applications. Compared to conventional methods, all these reactions went to completion in considerably shorter times at lower temperatures.     

Current-induced pseudospin polarization in silicene

The pseudospin polarization induced by an external electric field in silicene in the presence of weakly spinindependent impurities is considered theoretically in the linear response regime based on Green’s function method. We study the effects of the interplay between the sublattice potential and the intrinsic spin orbit coupling on the pseudospin polarization. We show that the pseudospin polarization perpendicular to the electric field is independent of the impurity parameter, while the pseudospin polarization in the direction of the electric field is sensitive to the impurity parameter. The dependences of the pseudospin polarizations on the chemical potential are studied.     

Physics and chemistry of silicene nano-ribbons

We review our recent discovery of silicene in the form of silicon nano-ribbons epitaxially grown on silver (1 1 0) or (1 0 0) surfaces, which paves the way for the growth of graphene-like sheets. We further draw some perspectives for this unique novel material upon mild hydrogenation.     

Electronic thermal Hall effect in silicene

We theoretically investigate the electronic thermal Hall effect in silicene via a discrete four-band model. Based on the linear response theory, a formalism to address the transverse thermal conductivity is developed. In the absence of an exchange field, the transverse thermal conductivity vanishes due to the time-reversal symmetry. The transverse conductivity becomes finite in the presence of an exchange field and exhibits several peaks with opposite signs. The peak values increase as the field becomes strong. However, as the temperature becomes high, the peak values begin to decay. The results may be helpful in exploring spin caloritronics based on silicene.     

Spin-polarized transport in multiterminal silicene nanodevices

The spin-polarized transport properties of multiterminal silicene nanodevices are studied using the tight binding model and Landauer–Buttier approach. We propose a four-terminal 2-shaped junction device and two types of three-terminal T-shaped junction devices, which are made of the crossing of a zigzag and an armchair silicene nanoribbon. If the electrons are injected into the metallic lead, the near-perfect spin polarization with 100% around the Fermi energy can be achieved easily at the other semiconducting leads. Thus the multiterminal silicene nanodevices can act as controllable spin filters.     

Controllable spin-dependent transport in silicene superlattice

Based on the transfer-matrix method, we theoretically investigate the spin-dependent transport properties in magnetic silicene superlattice in the presence of extrinsic Rashba spin–orbit interaction (RSOI). It is found that the spin transmission probability and spin conductivities can be efficiently controlled by the number of magnetic barriers. As the number of magnetic barriers increases, spin conductivities strongly decrease, and reduce to zero in the large on-site potential difference between A and B sublattices (Δ_z) region. The results indicate that a magnetic silicene superlattice exhibits a remarkable wavevector-dependent spin filtering effect. Also, the magnetoresistance (MR) ratio exhibits an oscillatory behavior with the Fermi energy. The MR ratio can be tuned by the Fermi energy, number of magnetic barriers and extrinsic RSOI. Specifically, in the presence of magnetic field the spin polarization can be observed, and increases by increasing the magnetic field.     

Electron-phonon coupling in armchair silicene nanoribbons

We report the effects of electron-phonon coupling on the charge density distribution of polarons in armchair nanoribbons of silicene by using an extended tight-binding model with lattice relaxation. The results show that the charge distribution in silicene nanoribbons is analogous to graphene and that the charge localization increases when the intensity of electron-phonon coupling also increases. We further show that silicene nanoribbons may be a conducting or semiconducting material, depending on both the width of the nanoribbon and the possibility of polaron formation. This contribution provides additional insight into the behavior of polarons in silicene nanoribbons, systems of great interest.     

Controllable spin transport in dual-gated silicene

Based on the dual-gated silicene, we have evaluated theoretically the spin-dependent transport in lateral resonant tunneling structure. By aligning the completely valley-polarized beam with spin-resolved well state in concerned structure, large spin polarization can be expected owing to spin-dependent resonant tunneling mechanism. Under the gate electric field modulation, the forming quantum well state can be externally manipulated, triggering further the emergence of externally-controllable spin polarization. Importantly, integrating the considered structure with a proper valley-filter, which might be constructed from valley-contrasting physics as that in graphene valleytronics, completely-polarized spin beam can also be attained without the assistance of ferromagnetic component, providing thus some profitable strategies to develop nonmagnetic spintronic devices residing on silicene.     

Current developments in silicene and germanene

Exploration of the unusual properties of the two‐dimensional materials silicene and germanene is a very active research field in recent years. This paper therefore reviews the latest developments, focusing both on the fundamental materials properties and on possible applications. (© 2016 WILEY‐VCH Verlag GmbH &Co. KGaA, Weinheim)     

Generation of valley pump currents in silicene

We propose a workable scheme for generating a bulk valley pump current in a silicene-based device which consists of two pumping regions characterized by time-dependent strain and staggered potentials, respectively. In a one-dimension model, we show that a pure valley current can be generated, in which the two valley currents have the same magnitude but flow in opposite directions. Besides, the pumped valley current is quantized and maximized when the Fermi energy of the system locates in the bandgap opened by the two pumping potentials. Furthermore, the valley current can be finely controlled by tuning the device parameters. Our results are useful for the development of valleytronic devices based on two-dimensional materials.     

Effects of heavy metal adsorption on silicene

Based on first‐principles calculations, we study the effects of heavy metal atoms (Au, Hg, Tl, and Pb) adsorbed on silicene. We find that the hollow site is energetically favorable in each case. We particulary address the question how the adsorption modifies the band structure in the vicinity of the Fermi energy. Our results demonstrate that the heavy metal adatoms result in substantial energy gaps and band splittings in the silicene sheet as long as the binding is strong, which, however, is not always the case. (© 2014 WILEY‐VCH Verlag GmbH &Co. KGaA, Weinheim)     

单层硅烯表面的CoPc分子吸附研究

由于低维材料表面上的单原子和分子具有丰富的物理化学性质,现已经成为量子器件及催化科学等领域的研究热点.单层硅烯在不同的衬底制备温度下,表现出丰富的超结构,这些超结构为实现有序的单原子或分子吸附提供了可靠的模板.利用原位硅烯薄膜制备,分子沉积,超高真空扫描隧道显微镜以及扫描隧道谱,本文研究了Ag(111)衬底上3种硅烯超结构((4×4),(■×■),(2■×2■))的电子态结构,表面功函数随超结构的变化,以及CoPc分子在这3种超结构硅烯上的吸附行为.研究结果表明,这3种超结构的硅烯具有类似的电子能带结构,且存在电子从Ag(111)衬底转移到硅烯上的可能性,从而导致硅烯的表面功函数增大,表面功函数在原子级尺度上的变化对分子的选择性吸附起着重要作用.此外,还观察到分子与硅烯的相互作用导致CoPc分子的电子结构发生对称性破缺.     

Chemical mechanical modification of nanodiamond in an aqueous system

The effect of chemical-mechanical modification (CMM) on the ζ potential and size distribution of nanodiamonds was studied. Results show a significant change in the functional groups on its surface after CMM treatment by the anionic surface modifier DN-10. The amount of hydroxyl groups decreases, and two peaks connected with the stretching vibration of carboxylate appear instead of those of carbonyl. The ζ potential goes up significantly, and the size drops to some extent. If treated further with CMM1, a new absorption peak appears at 1382.19 cm^?1 that is connected with the vibration of some distinctive functional groups that cause an increase in the ζ potential and a decrease in size.     

Anisotropic in-plane thermal conductivity in multilayer silicene

We systematically study thermal conductivity of multilayer silicene by means of Boltzmann Transportation Equation (BTE) method. We find that their thermal conductivity strongly depends on the surface structures. Thermal conductivity of bilayer silicene varies from 3.31 W/mK to 57.9 W/mK with different surface structures. Also, the $2\times 1$ surface reconstruction induces unusual large thermal conductivity anisotropy, which reaches 70% in a four-layer silicene. We also find that the anisotropy decreases with silicene thickness increasing, owing to the significant reduction of thermal conductivity in the zigzag direction and its slight increment in the armchair direction. Finally, we find that both the phonon-lifetime anisotropy and the phonon-group-velocity anisotropy contribute to the thermal conductivity anisotropy of multilayer silicene. These findings could be helpful in the field of heat management, thermoelectric applications involving silicene and other multilayer nanomaterials with surface reconstructions in the future.     

表面氢化双层硅烯的结构和电子性质

采用密度泛函理论(DFT)广义梯度近似GGA和HSB06方法研究了氢化双层硅烯(silicene)的结构和电子性质, 结果表明: 氢化后的双层硅烯可能存在三种稳定的构型, AA椅型、AB椅型和AA船型, 其中AA椅型和AB椅型结构最为稳定, 氢化后这三种稳定构型材料的性质由零带隙的半金属(semimetal)转变为禁带宽度分别为1.208, 1.437和1.111 eV 的间接带隙的半导体, 采用混合泛函HSB06计算修正得到的带隙分别为1.595, 1.785 和1.592 eV. 进一步分析了在双轴应变下氢化双层硅烯的带隙随应变的关系, 得到应变可以连续的调节材料的带隙宽度, 这些性质有可能应用于未来的纳米电子器件.