泡沫状二维复合材料的合成及超级电容器性能

利用蔗糖和乙醇作为碳源,以氯化镍高温还原形成的镍颗粒作为模板,制备了泡沫状石墨烯多孔材料。 继而以其作为载体,通过浸渍和高温热解法制备了泡沫状MoS₂/石墨烯二维复合材料。 通过扫描电子显微镜(SEM)、透射电子显微镜(TEM)、拉曼光谱、X射线衍射(XRD)等技术手段研究了复合材料的形貌、组成和结构。 循环伏安、恒流充放电和循环寿命测试均表明,该材料具有良好的超级电容器性能,质量比电容达203.5 F/g,面积比电容达280 mF/cm²,5000次恒流充放电循环后的电容保持率约80%。     

非共振圆偏振光作用下单层二硫化钼电子结构及其自旋/谷输运性质

基于紧束缚近似下的低能有效哈密顿模型和久保线性响应理论,研究了外部非共振圆偏振光作用下单层二硫化钼(MoS_2)电子结构及其自旋/谷输运性质.研究结果表明:单层MoS_2布里渊区K谷和K′谷附近自旋依赖子带间的能隙随着非共振右旋圆偏振光引起的有效耦合能分别线性增大和先减小后增大,随着非共振左旋圆偏振光引起的有效耦合能分别先减小后增大和线性增大,实现了系统能带结构有趣的半导体-半金属-半导体转变.此外,单层MoS_2在外部非共振圆偏振光作用下,呈现有趣的量子化横向霍尔电导和自旋/谷霍尔电导,自旋极化率在非共振右/左旋圆偏振光有效耦合能±0.79 eV附近达到最大并发生由正到负或由负到正的急剧转变,谷极化率随着非共振圆偏振光有效耦合能先增大后减小并在其绝对值0.79-0.87 eV范围内达到100%.因而,可以利用外部非共振圆偏振光将单层MoS_2调制成自旋/谷以及光电特性优异的新带隙材料.     

层数变化对堆叠生长的MoS_(2(1-x))Se_(2x)电子结构的影响

二维过渡金属硫化物因其独特的光电特性在多功能光电器件方面具有广泛的应用前景.为了进一步拓展其在微纳光电子器件方面的应用范围,并提高器件性能,人们开展了通过合金手段改变端组分材料配比实现对二维半导体材料带隙调控的带隙工程以及调控生长条件改变材料形貌和结构的缺陷工程研究.本文利用光学、原子力和扫描电子显微镜等设备以及拉曼和光致发光光谱等手段对由化学气相沉积法生长出来的堆叠状MoS_(2(1-x))Se_(2x)合金的性质进行了研究.不同于大多数单层或少层MoS_(2(1-x))Se_(2x)合金的情况,堆叠生长的阶梯状MoS_(2(1-x))Se_(2x)合金材料在厚度从2.2 nm (约3层)一直增加到5.6 nm (约7层)时都显出了较强的发光特性,甚至在100 nm厚时,样品的发光谱线仍具有两个发光峰.两个激子发光峰分别来源于自旋轨道耦合造成的价带劈裂.随着厚度的增加,两个峰都逐渐红移,显示了合金掺杂时的能带弯曲效应.拉曼光谱给出了类MoS_2和类MoSe_2两套振动模.随着厚度的增加,拉曼峰位几乎不移动,但面内的两个振动模E_(2g(Mo-Se))和E_(2g(Mo-s))逐渐显现并增强.显然缺陷和应力是影响堆叠生长MoS_(2(1-x))Se_(2x)合金样品电子结构的主要因素,这为特殊功能器件的制备和可控缺陷工程的研究提供了有益的参考.     

硅表面电沉积MoS2薄膜及其微观摩擦性能研究

以单晶硅片为基片,采用电化学沉积工艺通过阴极还原硫代钼酸根制备MoS2薄膜,利用光学显微镜、扫描电子显微镜、X射线衍射仪、俄歇电子能谱仪以及原子力显微镜表征薄膜结构,并研究其微观摩擦磨损性能.结果表明:所制备的薄膜为纳米/亚微米厚度,表面光滑致密,结构为非晶态,由钼、硫和氧元素构成;微米厚度的薄膜表面粗糙度增加,薄膜易开裂,结合性差;沉积MoS2薄膜的硅表面的最小摩擦力约为原始硅表面的1/2;沉积MoS2可以使硅表面的粘着能减少50%左右,从而使其微观摩擦力降低.     

二维MoS2/WSe2异质结的光电性能研究

近年来基于二维半导体过渡金属硫族化合物如MoS₂的光电晶体管被广泛研究。虽然基于单层MoS₂的光电探测器表现出较高的响应度,但是其较低的载流子迁移率也限制了响应时间,约在秒量级。二维半导体的相互堆垛可以形成具有低缺陷态且空间均匀的范德华异质结构,是提高二维光电探测器性能的有效途径。基于此本文通过机械剥离转移法构筑MoS₂/WSe₂垂直pn异质结,其较强的空间电荷区能有效地分离光生载流子,所以在自驱动状态下仍具有较好的光电探测能力,光响应度和探测率分别达到2.12×10³ A/W和2.33×10¹¹ Jones,同时极大地缩短了响应时间,响应时间达到40 ms。这种二维异质结器件制备方法简易,性能优异,在光电子领域具有广阔的应用前景。     

缺陷对单层MoS2电子结构的影响

为了研究缺陷对单层MoS2的电子结构, 本文基于密度泛函理论框架下的第一性原理, 采用数值基组的方法计算了MoS2的Mo位缺陷、S位缺陷的能带结构和态密度.结果发现：Mo位缺陷、S位缺陷的MoS2的能带结构中的价带顶与导带底都在Q点, 为直接带隙材料; 其中Mo位缺陷体的禁带区域都出现5条新能级, S位缺陷体的禁带区域出现了3条新能级; 缺陷体能带结构的能量下降与体系中未成键的电子有关.对于态密度而言, Mo位缺陷体的费米能级处出现了峰值, 表明Mo位缺陷会对其光电性质带来影响.同时分析电荷分布发现, Mo缺陷周围存在着负电荷聚集的现象, S缺陷周围存在正电荷聚集的现象.     

Growth behaviors and emission properties of Co-deposited MAPbI3 ultrathin films on MoS2

Hybrid organic-inorganic perovskite thin films have attracted much attention in optoelectronic and information fields because of their intriguing properties. Due to quantum confinement effects, ultrathin films in nm scale usually show special properties. Here, we report on the growth of methylammonium lead iodide (MAPbI₃) ultrathin films via co-deposition of PbI₂ and CH₃NH₃I (MAI) on chemical-vapor-deposition-grown monolayer MoS₂ as well as the corresponding photoluminescence (PL) properties at different growing stages. Atomic force microscopy and scanning electron microscopy measurements reveal the MoS₂ tuned growth of MAPbI₃ in a Stranski-Krastanov mode. PL and Kelvin probe force microscopy results confirm that MAPbI₃/MoS₂ heterostructures have a type-II energy level alignment at the interface. Temperaturedependent PL measurements on layered MAPbI₃ (at the initial stage) and on MAPbI₃ crystals in averaged size of 500 nm (at the later stage) show rather different temperature dependence as well as the phase transitions from tetragonal to orthorhombic at 120 and 150 K, respectively. Our findings are useful in fabricating MAPbI₃/transition-metal dichalcogenide based innovative devices for wider optoelectronic applications.     

Electronic Structure of the Low-Lying States of the Triatomic MoS2 Molecule: The Building Block of 2D MoS2

Molybdenum disulfide (MoS₂) is the building component of 1D-monolayer, 2D-layered nanosheets and nanotubes having many applications in industry, and it is detected in various molecular systems observed in nature. Here, the electronic structure and the chemical bonding of sixteen low-lying states of the triatomic MoS₂ molecule are investigated, while the connection of the chemical bonding of the isolated MoS₂ molecule to the relevant 2D-MoS₂, is emphasized. The MoS₂ molecule is studied via DFT and multireference methodologies, i. e., MRCISD(+Q)/aug-cc-pVQZ(−PP)_Mo. The ground state, ³B₁, is bent (Mo−S=2.133 Å and ϕ(SMoS)=115.9°) with a dissociation energy to atomic products of 194.7 kcal/mol at MRCISD+Q. In the ground and in the first excited state a double bond is formed between Mo and each S atom, i. e., . These two states differ in which d electrons of Mo are unpaired. The Mo−S bond distances of the calculated states range from 2.108 to 2.505 Å, the SMoS angles range from 104.1 to 180.0°, and the Mo−S bonds are single or double. Potential energy curves and surfaces have been plotted for the ³B₁, ⁵A₁ and ⁵B₁ states. Finally, the low-lying septet states of the triatomic molecule are involved in the material as a building block, explaining the variety of its morphologies.