单层正三角锯齿型石墨烯量子点的电子结构和磁性

采用基于密度泛函理论的广义梯度近似(GGA),对不同尺寸(N=2—11)的单层正三角锯齿型石墨烯量子点(Z_N -GNDs)的结构进行优化,得到与实验数据较好符合的晶格常数,进一步计算得到不同尺寸下体系的自旋多重度、磁矩、电子态密度以及自旋电子密度.结果表明:所有体系都呈现金属性,在尺寸较小的体系中量子尺寸效应对电子结构的影响比较明显;与单层石墨烯片一样,sp²杂化作用和非键态电子在量子点中仍起到非常重要的作用;费米能级上有自旋向上的电子分布,体系的 关键词： 石墨烯 量子点 电子结构 磁性     

点缺陷扶手型石墨烯量子点的电子性质研究

基于有限差分方法, 数值求解了Dirac方程, 研究了垂直磁场下的点缺陷扶手型 石墨烯 量子点的能谱结构, 分析了尺寸大小对带隙的影响. 与无磁场时具有一定带隙 (带隙的大小与半径成反比) 的量子点相比, 在外加有限磁场下, 能谱中出现朗道能级, 最低朗道能级能量为零并与磁场强度无关, 并且朗道能级的简并度随着磁场的增加而增加. 进一步的计算表明, 最低朗道能级的简并度与磁场成线性关系, 与半径的平方成线性关系. 本文工作对基于石墨烯量子点的器件设计具有一定的指导意义.     

尺寸分布对量子点激发态发光性质的影响

采用有效质量近似方法研究了量子点的激发态光致发光峰的展宽问题. 对尺寸不均匀分布下量子点各能级发光峰与平均尺寸量子点发光峰的能量偏差进行了计算，定性地描述了尺寸分布对量子点基态和激发态发光峰展宽的影响. 研究表明，量子点的高度、直径以及体积等不均匀分布使量子点具有不同的垂直、平面方向的量子束缚. 这两种量子限制的相互作用决定了量子点激发态发光峰的宽度相对于基态发光峰的大小. 在各种不同性质的尺寸分布下，量子点激发态发光峰的展宽有可能大于、等于或小于基态发光峰的展宽. 关键词： 量子点 尺寸分布 激发态     

溶剂对石墨烯量子点荧光性质的影响

采用柠檬酸热解法制备了石墨烯量子点(GQDs),研究了非极性溶剂戊烷,极性溶剂乙醇、丙酮、乙二醇对GQDs荧光性质的影响。透射电子显微镜(TEM)和原子力显微镜(AFM)图像表明,制备的GQDs尺寸分布在2~12 nm(平均尺寸为4.9 nm),分散均匀,高度分布在0.5~2 nm。吸收光谱表明,GQDs具有明显的紫外吸收特性,吸收峰位于259 nm和274 nm。光致发光谱表明,GQDs的发光具有明显的溶剂依赖性。GQDs在极性溶剂乙醇、丙酮、乙二醇中,发光峰的位置依赖于激发波长,发射波长在可见光区。而在非极性溶剂戊烷中,GQDs表现出对激发波长不依赖的荧光性能,且发射波长在近紫外。     

抛物量子点中强耦合磁双极化子内部激发态性质

基于Lee-Low-Pines幺正变换,采用Pekar类型变分法研究了抛物量子点中强耦合磁双极化子的内部激发态性质,当考虑自旋和外磁场影响时,推导出二维量子点中强耦合磁双极化子基态的能量E0,声子平均数ˉN0以及第一激发态的能量E1,声子平均数ˉN1随量子点受限强度ω0,介电常数比η,电子-声子耦合强度α和磁场的回旋共振频率ωC的变化规律.结果表明,磁双极化子的基态能量E0和第一激发态能量E1由两电子的单粒子能量E E,两电子间库仑相互作用能E C,电子自旋与磁场相互作用能E s和电子-声子相互作用能E e-ph四部分组成;单粒子"轨道"运动与磁场相互作用导致了第一激发态能级E1分裂为E(1+1)1,E(1-1)1两条,而电子自旋-磁场相互作用的效应又使基态和第一激发态的各能级均产生了三条"精细结构";ˉN0和ˉN1随ω0,α和ωc的增加而增大,E e-ph的取值总是小于零,其绝对值随α,ω0和ωc的增加而增大;电子-声子相互作用的效应是束缚态磁双极化子形成的有力因素,而限定势和电子之间的库仑排斥能的存在不利于束缚态磁双极化子的形成;能量为E(1-1)1的磁双极化子要比能量为E(1+1)1的磁双极化子更容易且更稳定地处于束缚态.     

量子点中极化子的内部激发态性质

采用Huybrechts线性组合算符和幺正变换方法研究了抛物量子点中的强、弱耦合极化子的激发态性质。分别导出强、弱耦合情况下,抛物量子点中的极化子的第一内部激发态能量、激发能量、共振频率与量子点的有效受限长度和电子-声子耦合强度的关系。数值计算结果表明,量子点中弱耦合和强耦合极化子的内部激发态能量、激发能量和共振频率都随量子点的有效受限长度的减小而迅速增大。弱耦合极化子的第一内部激发态能量随电子-声子耦合强度的增加而减少;而强耦合极化子的振动频率随量子点的有效受限长度的减小而迅速增加。弱耦合极化子的第一内部激发态能量、激发能量和共振频率随电子-声子耦合强度的增加而减小。     

非对称量子点中强耦合磁极化子激发态的性质

采用线性组合算符和幺正变换方法,研究非对称量子点中强耦合磁极化子的激发态性质。导出强耦合磁极化子的第一内部激发态能量、激发能量和从第一内部激发态到基态的跃迁谱线频率随量子点的横向和纵向有效受限长度、磁场的回旋频率和电子-声子耦合强度的变化关系。数值计算结果表明：第一内部激发态能量、激发能量和跃迁谱线频率随磁场的回旋频率和电子-声子耦合强度的增加而增大.随量子点的横向和纵向有效受限长度的减小而迅速增大,表现出奇特的量子尺寸效应。     

量子点中弱耦合束缚极化子的内部激发态性质

采用线性组合算符和幺正变换方法研究库仑束缚势对量子点中弱耦合束缚极化子激发态性质的影响。计算了束缚极化子的振动频率、第一内部激发态能量、激发能量和共振频率随量子点的有效受限长度,电子-声子耦合强度和库仑束缚势的变化关系。结果表明:量子点中弱耦合束缚极化子的振动频率、第一内部激发态能量、激发能量和共振频率随量子点的有效受限长度的减少而迅速增大,随库仑束缚势的增加而增大。     

石墨烯量子点:制备及检测乙醇-水溶液组分

采用改进的非完全脱水碳化方法制备石墨烯量子点.产物尺寸约6 nm,激发峰355 nm,发射峰458 nm.基于乙醇对石墨烯锯齿边质子化的抑制效应,发现可通过石墨烯量子点荧光光强检测乙醇-水混合溶液组分.在0.01-100%范围内,乙醇体积百分比与发射峰光强增量呈线性关系.本研究为制备石墨烯量子点提供参考,提出了简易的较宽范围的乙醇水溶液含量检测方法 .     

Quantum confinement in graphene quantum dots

By performing density functional theory calculations, we studied the quantum confinement in charged graphene quantum dots (GQDs), which is found to be clearly edge and shape dependent. It is found that the excess charges have a large distribution at the edges of the GQD. The resulting energy spectrum shift is very nonuniform and hence the Coulomb diamonds in the charge stability diagram vary irregularly, in good agreement with the observed nonperiodic Coulomb blockade oscillation. We also illustrate that the level statistics of the GQDs can be described by a Gaussian distribution, as predicted for chaotic Dirac billiards.

     

Optical properties of geometrically optimized graphene quantum dots

We derive effective tight-binding model for geometrically optimized graphene quantum dots and based on it we investigate corresponding changes in their optical properties in comparison to ideal structures. We consider hexagonal and triangular dots with zigzag and armchair edges. Using density functional theory methods we show that displacement of lattice sites leads to changes in atomic distances and in consequence modifies their energy spectrum. We derive appropriate model within tight-binding method with edge-modified hopping integrals. Using group theoretical analysis, we determine allowed optical transitions and investigate oscillatory strength between bulk–bulk, bulk–edge and edge–edge transitions. We compare optical joint density of states for ideal and geometry optimized structures. We also investigate an enhanced effect of sites displacement which can be designed in artificial graphene-like nanostructures. A shift of absorption peaks is found for small structures, vanishing with increasing system size.     

An approach to controlling the fluorescence of graphene quantum dots: From surface oxidation to fluorescent mechanism

We report a facile method of synthesizing graphene quantum dots（GQDs） with tunable emission. The as-prepared GQDs each with a uniform lateral dimension of ca. 6 nm have fine solubility and high stability. The photoluminescence mechanism is further investigated based on the surfacestructure and the photoluminescence behaviors. Based on our discussion, the green fluorescence emission can be attributed to the oxygen functional groups, which could possess broad emission bands within the π –π ＊ gap. This work is helpful to explain the vague fluorescent mechanism of GQDs, and the reported synthetic method is useful to prepare GQDs with controllable fluorescent colors.     

基于石墨烯-钙钛矿量子点场效应晶体管的光电探测器

以等离子增强化学气相沉积法制备的石墨烯作为导电沟道材料,将其与无机CsPbI_3钙钛矿量子点结合,设计并制备了石墨烯-钙钛矿量子点场效应晶体管光电探测器.研究和分析了石墨烯作为场效应晶体管的电学特性及其与钙钛矿量子点结合作为光电探测器的光电特性.结果表明,石墨烯在场效应晶体管中表现出良好的电学性质,其与钙钛矿量子点的结合对波长为400 nm的光辐射具有明显的光响应,在光强为12μW时器件光生电流最大为64μA,响应率达6.4 A·W~(-1),对应的光电导增益和探测率分别为3.7×10~4,6×10~7Jones(1 Jones=1 cm·Hz~(1/2)·W~(-1)).     

State-filling and magneto-photoluminescence of excited states in InGaAs/GaAs self-assembled quantum dots

We present the first radiative lifetime measurements and magneto-photoluminescence results of excited states in InGaAs/GaAs semiconductor self-assembled quantum dots. By increasing the photo-excitation intensity, excited state interband transitions up ton= 5 can be observed in the emission spectrum. The dynamics of the interband transitions and the inter-sublevel relaxation in these zero-dimensional energy levels lead to state-filling of the lower-energy states, allowing the quasi-Fermi level to be raised by more than 200 meV due to the combined large inter-sublevel spacing and the low density of states. The decay time of each energy level obtained under various excitation conditions is used to evaluate the inter-sublevel thermalization time. Finally, the emission spectrum of the dots filled with an average of about eight excitons is measured in magnetic fields up to 13 Tesla. The dependences of the spectrum as a function of carrier density and magnetic field are compared to calculations and interpreted in terms of coherent many-exciton states and their destruction by the magnetic field.     

Transmission phase lapses at zero energy in graphene quantum dots

We address theoretically the electronic transport through graphene quantum dots with the emphasis on the transmission phase. Analytical and numerical results are presented regarding the existence – or not – of a π lapse of the transmittance phase (and, consequentially, a Fano zero in the transmittance) at the charge neutrality point. A simple universal criterium is found, the phase lapses being always present if the contact sites belong to the same sub‐lattice. (© 2014 WILEY‐VCH Verlag GmbH &Co. KGaA, Weinheim)