Molecular beam epitaxy growth and characterization of self-assembled InAs quantum dots on (1 0 0) InAlAs/InP substrates

Self-assembled InAs quantum dots (QDs) on In_0.52Al_0.48As layer lattice matched to (1 0 0) InP substrates have been grown by molecular beam epitaxy (MBE) and evaluated by transmission electron microscopy (TEM) and photoluminescence (PL). TEM observations indicate that defect-free InAs QDs can be grown to obtain emissions over the technologically important 1.3–1.55 μm region. The PL peak positions for the QDs shift to low energy as the InAs coverage increases, corresponding to increase in QD size. The room temperature PL peak at 1.58 μm was observed from defect-free InAs QDs with average dot height of 3.6 nm.     

Advances in photonic crystals with MEMS and with semiconductor quantum dots

We discuss photonic crystals (PCs) with a microelectromechanical system (MEMS) and semiconductor quantum dots (QDs) as novel classes of PC devices. Integration of MEMS structures into PC devices enables one to realize several kinds of functional devices, such as modulators, switches, and tunable filters for highly integrated photonic circuits. We describe the basic concept of MEMS-integrated PC devices and show numerical and experimental demonstrations of MEMS-integrated functional PC devices. On the other hand, QDs are promising candidates for active media in PC devices. Spontaneous emission control of QD emission in PC nanocavities is especially important for novel optoelectronic devices and quantum information devices. In PC nanocavities, the interaction between QD excitons and photons is enhanced dramatically. The control of spontaneous emission spectrum and the enhancement of the luminescence intensity of InAs QDs by PC nanocavities are demonstrated at telecommunication wavelengths. The Purcell effect for ensemble and single QDs in PC nanocavities are also discussed.     

2018年5期 电子期刊

研究了不同Mn/Pb量比的Mn掺杂CsPbCl₃（Mn：CsPbCl₃）钙钛矿量子点的发光性质。Mn/Pb的量比增加引起的Mn²⁺发光峰的红移,被认为是来源于高浓度Mn²⁺掺杂下的Mn²⁺-Mn²⁺对。进一步研究了Mn：CsPbCl₃量子点的发光效率与Mn/Pb的量比之间的关系,发现随着量比达到5：1时,其发光效率明显下降。这种发光效率下降是由于Mn掺杂浓度引起的发光猝灭。Mn：CsPbCl₃量子点的变温发光光谱证实,随着温度的升高,Mn离子发光峰蓝移,线宽加宽,但其发光强度明显增加。     

InAs/GaAs量子点1.3 μm单光子发射特性

采用双层耦合量子点的分子束外延生长技术生长了InAs/GaAs量子点样品,把量子点的发光波长成功地拓展到1.3 μm.采用光刻的工艺制备了直径为3 μm的柱状微腔,提高了量子点荧光的提取效率.在低温5 K下,测量得到量子点激子的荧光寿命约为1 ns;单量子点荧光二阶关联函数为0.015,显示单量子点荧光具有非常好的单光子特性;利用迈克耳孙干涉装置测量得到单光子的相干时间为22 ps,对应的谱线半高全宽度为30 μeV,且荧光谱线的线型为非均匀展宽的高斯线型.     

Stability and luminescence properties of CsPbBr3/CdSe/Al core-shell quantum dots

To improve the stability and luminescence properties of CsPbBr₃ QDs, we proposed a new core-shell structure for CsPbBr₃/CdSe/Al quantum dots (QDs). By using a simple method of ion layer adsorption and a reaction method, CdSe and Al were respectively packaged on the surface of CsPbBr₃ QDs to form the core-shell CsPbBr₃/CdSe/Al QDs. After one week in a natural environment, the photoluminescence quantum yields of CsPbBr₃/CdSe/Al QDs were greater than 80%, and the PL intensity remained at 71% of the original intensity. Furthermore, the CsPbBr₃/CdSe/Al QDs were used as green emitters for white light-emitting diodes (LEDs), with the LEDs spectrum covering 129% of the national television system committee (NTSC) standard color gamut. The core-shell structure of QDs can effectively improve the stability of CsPbBr₃ QDs, which has promising prospects in optoelectronic devices.     

Optimum Quantum Yield of the Light Emission from 2 to 10 nm Hydrosilylated Silicon Quantum Dots

Optimizing the light‐emitting efficiency of silicon quantum dots (Si QDs) has been recently intensified by the demand of the practical use of Si QDs in a variety of fields such as optoelectronics, photovoltaics, and bioimaging. It is imperative that an understanding of the optimum light‐emitting efficiency of Si QDs should be obtained to guide the design of the synthesis and processing of Si QDs. Here an investigation is presented on the characteristics of the photoluminescence (PL) from hydrosilylated Si QDs in a rather broad size region (≈2–10 nm), which enables an effective mass approximation model to be developed, which can very well describe the dependence of the PL energy on the QD size for Si QDs in the whole quantum‐confinement regime, and demonstrates that an optimum PL quantum yield (QY) appears at a specific QD size for Si QDs. The optimum PL QY results from the interplay between quantum‐confinement effect and surface effect. The current work has important implications for the surface engineering of Si QDs. To optimize the light‐emission efficiency of Si QDs, the surface of Si QDs must be engineered to minimize the formation of defects such as dangling bonds at the QD surface and build an energy barrier that can effectively prevent carriers in Si QDs from tunneling out.     

衬底钝化处理对CsPbBr3 量子点薄膜发光稳定性影响

钙钛矿量子点因具有发光谱线窄、发光效率高、发光波长可调谐等优异的光学性能,在照明、显示、激光和太阳能电池等领域得到了广泛研究。然而,钙钛矿材料的稳定性问题,一直制约着其在光电器件中的应用。其中,钙钛矿材料在空气中受潮易分解的不稳定性尤为突出,这将严重影响其发光性质。为此,研究人员采用多种手段来改善钙钛矿材料的稳定性。目前,常见的方法是将一些具有疏水性的聚合物材料（例如POSS,PMMA等）引入到钙钛矿纳米晶中,或将钙钛矿纳米晶嵌入到介孔二氧化硅材料中,避免钙钛矿纳米晶暴露于空气中破坏其结构,以此来增强钙钛矿材料的发光稳定性。此外,钝化处理钙钛矿纳米晶表面,也是改善钙钛矿发光稳定性的一种常用方法。这些方法虽然在一定程度上可以改善钙钛矿的发光稳定性,但是在与有机物合成的过程中不免会引入其他有机官能团,介孔二氧化硅的引入,其处理方式相对复杂,而对钙钛矿纳米晶表面的钝化处理会破坏材料的原有结构。以上问题,都会影响钙钛矿的发光性质,不利于其在光电器件中的应用。硅（Si）具有低成本、大尺寸、高质量、导电好等优点,常被选作钙钛矿量子点光电器件的衬底材料。但是,由于Si衬底长时间暴露于空气,其表面易形成一层具有硅烷醇基团（Si-OH）的亲水性薄膜,这将对硅基钙钛矿器件的稳定性产生影响。因此,对Si表面进行钝化处理,破坏其表面Si-OH键,可以降低衬底表面的亲水性,增强疏水性,从而提高钙钛矿材料在器件中的稳定性。本研究使用氢氟酸（HF）对Si衬底表面进行钝化处理,发现钝化处理后的Si衬底表面与水的接触角由50.4°逐渐增大至87.7°,表明Si衬底表面由亲水性逐渐转变为疏水性。利用场致发射扫描电子显微镜(FE-SEM)测试发现,钝化处理后的Si衬底表面变粗糙,并且其表面上的CsPbBr₃量子点(CsPbBr₃ QDs)相对于未处理表面的分散性较好。利用光致发光(PL)光谱研究不同钝化处理时间的Si衬底表面上的CsPbBr₃ QDs薄膜的发光性质。其中,处理与未处理的Si衬底表面上CsPbBr₃QDs薄膜的PL积分强度随功率变化拟合值分别为1.12和1.203,表明其发光机制为激子发光。温度依赖性的PL光谱分析显示,随着温度的升高（10～300 K）,由于晶格热膨胀使CsPbBr₃ QDs带隙增大,发光峰位逐渐蓝移。并且,随着衬底钝化处理时间的增加,CsPbBr₃ QDs薄膜的发光热稳定性逐渐增强,最佳热稳定性可达220 K。而时间依赖性的PL光谱则进一步说明,钝化处理后的Si衬底表面CsPbBr₃QDs薄膜发光的时间稳定性逐渐增强,最高发光时间稳定性可达15 d。因此,通过简单而有效的对Si衬底表面进行钝化处理,可以有效减少了Si表面亲水基团,提高CsPbBr₃QDs薄膜的发光稳定性,为增强钙钛矿量子点在光电器件中的稳定性应用提供了新的研究思路。     

金属离子修饰的ZnS/PAMAM纳米复合材料的荧光性能研究

用荧光分光光度法研究了Zn2+,Mn2+,Cd2+,Na+,K+,Ag+,Cu2+和Pb2+等金属离子修饰的ZnS/PAMAM树形分子纳米复合材料的荧光发射性能。结果表明：不同金属离子修饰效果不同。Zn2+,Mn2+和Cd2+修饰后,ZnS/PAMAM树形分子纳米复合材料的荧光发射强度有不同程度提高;Ag+,Cu2+和Pb2+的修饰对荧光有不同程度的猝灭作用;而Na+和K+的修饰对荧光发射无明显影响。与修饰前相比,Cd2+离子修饰的ZnS/PAMAM树形分子纳米复合材料标记的潜指纹发射的蓝色荧光更加明亮,与背景反差更加明显。这对提高潜指纹的显现精度和准确率有很好的借鉴价值。     

Magneto-optical properties and exciton dynamics in diluted magnetic semiconductor nanostructures

Nanostructures of diluted magnetic semiconductors were fabricated to study novel magneto-optical properties that are derived from quantum confined band electrons interacting with magnetic ions. Quantum dots (QDs) of Cd_0.97Mn_0.03Se were grown by the self-organization on a ZnSe substrate layer. QDs of Zn_0.69Cd_0.23Mn_0.08Se and quantum wires (QWRs) of Cd_0.92Mn_0.08Se and Zn_0.69Cd_0.23Mn_0.08Se were fabricated by the electron beam lithography. A single quantum well (QW) of ZnTe/Zn_0.97Mn_0.03Te and double QWs of Cd_0.95Mn_0.05Te–CdTe were grown by molecular beam epitaxy. Magneto-optical properties and the formation and relaxation dynamics of excitons were investigated by ultrafast time-resolved photoluminescence (PL) spectroscopy. Excitons in these nanostructures were affected by the low-dimensional confinement effects and the interaction with magnetic ion spins. The exciton luminescence of the Cd_0.97Mn_0.03Se QDs shows the confined exciton energy due to the dot size of 4–6 nm and also shows marked increase of the exciton lifetime with increasing the magnetic field. The QDs of Zn_0.69Cd_0.23Mn_0.08Se fabricated by the electron beam lithography display narrow exciton PL spectrum due to the uniform shape of the dots. The exciton luminescence from the QWRs of Cd_0.92Mn_0.08Se and Zn_0.69Cd_0.23Mn_0.08Se shows the influence of the one-dimensional confinement effect for the exciton energy and the luminescence is linearly polarized parallel to the wire direction. The transient PL from the ZnTe/Zn_0.97Mn_0.03Te QWs displays, by the magnetic field, the level crossing of the exciton spin states of the nonmagnetic and magnetic layers and the spatial spin separation for the excitons. Cd_0.95Mn_0.05Te–CdTe double QWs show the injection of the spin polarized excitons from the magnetic well to the nonmagnetic QW.     

UV-induced two-photon absorption in BiB3O6 single crystals

We show that BiB₃O₆ (BiBO) crystals, well known for their excellent second harmonic generation (SHG) properties, may also be of interest for third-order optical phenomena, particularly for two-photon absorption (TPA). Photoinduced TPA measurements were performed under illumination of excimer Xe–F laser (λ = 217 nm) as a photoinducing (pumping) beam. It created a thin surface layer (about 85 nm) that was a source of the observed photoinduced TPA. Raman shifted Nd-YAG laser radiation (λ = 1.9 μm) as well as its second and fourth harmonics (λ = 950 and λ = 475 nm, respectively) were used as fundamental (probing) beams of the TPA. The highest values of the TPA β coefficient were achieved for a polarization of the pumping light directed along crystallographic axis b. Quantum chemical simulations indicate on substantial contribution of UV-induced electron–phonon anharmonicity to the observed TPA. The obtained values of TPA coefficients indicate a possibility of using BiBO crystals as UV-operated optical limiters in a wide spectral range.     

Decay lifetime and evolution of semiconductor quantum dots in photonic crystals

Spontaneous emission from GaAs/AlGaAs quantum dots (QDs) embedded in photonic crystals with a narrow photonic band gap is studied theoretically. The results show that the decay lifetime is very sensitive to the sizes of QDs, and both inhibited and accelerated emission can occur, which had been indicated in a previous experiment. The Weisskopf–Wigner approximation, good for atoms and molecules, may be incorrect for QDs. A damped Rabi oscillation of the excited state with the transition frequency outside the photonic band gap may appear, which is impossible for atoms and molecules.     

Modified Spontaneous Emission from Dye Molecules inside a Photonic Crystal Microcavity

We fabricate a photonic crystal microcavity containing Alq3 in a sandwiched structure by the self-assemble method. The angle-dependent photoluminescence （PL） spectra and the variation of the PL lifetime demonstrate the effect of the photonic band gap on the spontaneous emission of Alq3 in the photonic crystals.     

Manipulating light flow with one-dimensional photonic crystals of an electromagnetically induced transparency medium

The band structures and equifrequency contours of one-dimensional photonic crystals (PCs), which consist of an electromagnetically induced transparency (EIT) medium and a common dielectric medium, can be dramatically changed by tuning the coupling field intensity (or coupling Rabi frequency, CRF) of the EIT medium. It is found that for a probe light at a fixed frequency, either positive or negative refraction in the EIT PC can be realized with a proper CRF. The behavior of a Gaussian beam (probe light) obliquely incident on such an EIT PC slab is simulated numerically. The probe light beam transmitted from the slab can be shifted transversely in a large range, and negative refraction enhances this effect. The present scenario can be applied in some areas such as quantum optical and photonic device designs.     

轴向填充率渐变型二维光子晶体

提出了一种轴向填充率渐变型二维三角晶格方空气孔光子晶体,由锥形孔周期性排布而成,在第三维也就是沿空气孔的轴向,空气孔的尺寸连续改变,实现了填充率渐变,填充率f范围为0.700～0.866。经过模拟,在归一化波长(λ/a)的1.43～2.71和3.41～4.00波段,轴向填充率渐变型光子晶体可以将光向填充率小的方向偏折,具有选光功能。采用电化学腐蚀与MEMS工艺相结合的方式,在p型(100)硅基底上制作了轴向填充率渐变型二维三角晶格方孔光子晶体,整个孔的填充率f在0.800～0.866范围内。     

Effect of Mercaptocarboxylic Acids on Luminescent Properties of CdTe Quantum Dots

CdTe quantum dots (QDs) were prepared in an aqueous solution using various mercaptocarboxylic acids, such as 3-mercaptopropionic acid (MPA) and thioglycolic acid (TGA), as stabilizing agents. The experimental result indicated that these stabilizing agents played an important role for the properties of the QDs. Although both TGA and MPA-capped CdTe QDs exhibited the tunable photoluminescence (PL) from green to red color, the TGA-capped QDs revealed a higher PL quantum yield (QY) up to 60% than that of MPA-capped QDs (up to 50%) by using the optimum preparation conditions, such as a pH value of ~11.2 and a TGA/Cd molar ratio of 1.5. PL lifetime measurements indicate that the TGA-capped QDs exhibited a short average lifetime while the MPA-capped QDs revealed a long one. Furthermore, the average lifetime of the TGA-capped QDs increased with the increase of the QDs size, while a decreased lifetime for the MPA-capped QDs was obtained. This means that the PL lifetime depended strongly on the surface state of the CdTe QDs. These results should be utilized for the preparation and applications of QDs.     

PbSe量子点荧光匹配气体吸收光谱方法研究

PbSe量子点(PbSe-QDs)是红外波段的典型纳米材料,其具有大的玻尔半径、小的体材料禁带宽度(玻尔半径是46 nm,体材料禁带宽度是0.28 eV),因此,在近红外区域,PbSe-QDs具有强大的尺寸受限效应和较高的量子产出率。本文对不同尺寸的PbSe量子点的荧光光谱特性进行了研究,提出了一种通过调节PbSe量子点的量子尺寸匹配气体吸收光谱的方法。采用配位溶剂的方法制备了尺寸为4.6和6.1 nm的PbSe量子点,将该PbSe量子点沉积到GaN发光芯片上并经过紫外光照处理和固化后制成了光致发光的近红外光源,其中4.6 nm的PbSe-QDs的沉积厚度为671.5 μm,而6.1 nm的PbSe-QDs的沉积厚度为48 μm。将制成的近红外光源应用到C₂H₂气体和NH₃气体的检测实验中,实验结果表明,通过改变PbSe量子点的尺寸可以调节光源光致发光峰的位置,从而覆盖目标气体在近红外波段的吸收谱线。4.6 nm的光源发射光谱包含了1 500～1 550 nm之间的C₂H₂气体的全部的吸收谱;6.1 nm的光源发射光谱包含了1 900～2 060 nm之间的NH₃气体的全部的吸收谱。这种利用PbSe量子点尺寸的可调性匹配对应气体吸收谱的方法是可行和有效的,具有广阔的应用前景。     

用一维光子带隙结构增强硫化镉双光子吸收研究

用真空镀膜方法制备了含有单个CdS缺陷层的具有不同周期和结构参量的TiO2／SiO2一维光子晶体。用抽运一探测技术研究了CdS缺陷层的双光子吸收（TPA）现象。实验结果表明：一维光子晶体中CdS缺陷层的双光子吸收显著增强。不同周期和结构参量的一维光子晶体中CdS缺陷层的双光子吸收系数不同。双光子吸收的增强来源于由光局域化导致的缺陷层的电场强度的增加。缺陷层电场强度与一维光子晶体的结构有关,如周期,光子带隙的位置与宽度及缺陷模式等因素都会影响缺陷层电场强度。采用四分之一波长的高低折射率介质层和与入射波长匹配的缺陷模可以得到最大的缺陷层电场强度。     

径向偏振光下的长焦、紧聚焦表面等离子体激元透镜

表面等离子体激元透镜(plasmonic lens, PL)是一种通过激发和操控表面等离子体激元 (SPPs), 突破衍射极限, 实现亚波长紧聚焦的纳米光子器件. 如何实现高效率的紧聚焦及调控, 一直是研究PL的重点. 如果选取电矢量沿径向振动的径向偏振光作为PL的入射光, 可从各个方向激发SPPs, 提高紧聚焦的能量效率. 本文提出了一种在径向偏振光激发下的长焦深、长焦距、亚波长紧聚焦的表面等离子体激元透镜, 该透镜由中心T 形微孔、阶梯形同心环和同心环结构组成. 本文首先利用有限元方法数值分析了中心微孔-同心环结构透镜的聚焦特性, 结果显示径向偏振光由底部入射可高效激发SPPs, 并且中心微孔透射光与散射至自由空间的SPPs由于多光束干涉形成了紧聚焦. 为进一步压缩焦斑、增加焦距、加深焦深、改善透镜聚焦特性, 本文引入中心T形微孔-阶梯形同心环结构, 从而对阶梯表面的SPPs同时提供了相位调制和传播方向的控制. 经过参数优化, 该透镜结构实现了光斑焦深、半高宽、焦距分别是入射光波长的2.5倍、0.388 倍、3.22倍的亚波长紧聚焦; 而且该透镜具有结构紧凑、尺寸小、易于集成的优点, 满足了纳米光子学对于器件微型化和高度集成化的要求. 该研究结果在纳米光子集成、近场光学成像与探测、纳米光刻等相关领域具有潜在的应用价值.     

Fabrication of three‐dimensional photonic crystals in quantum‐dot‐based materials

Controlling spontaneous emission (SE) is of fundamental importance to a diverse range of photonic applications including but not limited to quantum optics, low power displays, solar energy harvesting and optical communications. Characterized by photonic bandgap (PBG) property, three‐dimensional (3D) photonic crystals (PCs) have emerged as a promising synthetic material, which can manipulate photons in much the same way as a semiconductor does to electrons. Emission tunable nanocrystal quantum dots (QDs) are ideal point sources to be embedded into 3D PCs towards active devices. The challenge however lies in the combination of QDs with 3D PCs without degradation of their emission properties. Polymer materials stand out for this purpose due to their flexibility of incorporating active materials. Combining the versatile multi‐photon 3D micro‐fabrication techniques, active 3D PCs have been fabricated in polymer‐QD composites with demonstrated control of SE from QDs. With this milestone novel miniaturized photonic devices can thus be envisaged.     

近红外波段InAs量子点结构与光学特性

采用分子束外延技术,分别在480,520℃的生长温度下,制备了淀积厚度2.7ML的InAs/GaAs量子点。用原子力显微镜对样品进行形貌测试和统计分布。结果表明,在相应的生长温度下,量子点密度分别为8.0×10¹⁰,5.0×10⁹cm^-2,提高生长温度有利于获得大尺寸的量子点,并且量子点按高度呈双模分布。结合光致发光谱的分析,在480℃的生长条件下,最近邻量子点之间的合并导致了量子点尺寸的双模分布;而在525℃的生长温度下,In偏析和InAs解析是形成双模分布的主要原因。