Guided mode lasing in ZnO nanorod structures

Quasi-two-dimensional arrays of nearly parallel hexagonal ZnO nanorods and a three-dimensional cylindrical microstructure consisting of ZnO nanorods have been grown by low pressure chemical vapor deposition (CVD) and carbothermal evaporation technologies, respectively. The technology ensures high optical quality of the produced nanostructures so as to act as a gain medium for stimulated emission in the ultraviolet spectral region in combination with high quality factor laser resonators. Multiple sharp lasing peaks were realized from the produced structures under nanosecond pulse optical excitation. The lasing peaks display successive onset and saturation with increasing excitation power density in accordance with the lasing behavior of guided modes in ZnO nanorods. The produced structures are expected to find applications in integrated nanoscale optoelectronics, photonics, and sensor technologies.     

利用金作为反射镜的氧化锌纳米棒光泵激光

通过水热法在溅射了一层金的Si片上生长了ZnO纳米棒。实验观察到ZnO纳米棒的室温光致发光谱中出现了强的紫外发射峰,同时还伴随有弱的缺陷相关的发射,这表明通过该种方法生长的ZnO纳米棒晶体质量较好。同时,通过光泵浦也观察到了ZnO纳米棒中的激光发射。当激发光功率密度超过阈值,且进一步增加时则出现多个发射峰,其积分强度随着激发功率密度的增大呈非线性增长,进一步表明存在受激发射。利用金属层作为反射镜可以进一步降低损耗,从而达到降低阈值的目的。     

Multiphoton route to ZnO nanowire lasers

With intense femtosecond laser excitation, multiphoton absorption-induced stimulated emission and laser emission in ZnO bulk crystal and nanowires have been demonstrated at room temperature. UV-stimulated emission peaks appeared in both bulk crystal and nanowires when the excitation exceeded certain thresholds, and a sharp lasing peak with a linewidth of ~0.5 nm was observed from ZnO nanowires. The emission properties were attributed to the band-edge emission of the recombination of carriers excited by two- and three-photon absorption processes in the wide-bandgap semiconductor.     

Multi-photon-pumped stimulated emission from ZnO nanowires: A time-resolved study

In this work, we study temporal evolution of multi-photon-pumped stimulated emission from ZnO nanowires. In addition to second harmonic generation, ultraviolet stimulated emission is observed in ZnO nanowires under femtosecond pulse excitation at 800 nm. Sharp emission peaks appear when excitation flux reaches a threshold of 80 mJ/cm², which can be interpreted as lasing action in self-formed nanowire microcavities. Temporal evolution of the emission captured by Kerr shutter technique shows strong excitation-power dependence. The dynamic trace of stimulated emission exhibits a fast decay with a lifetime about 4.5 ps at intermediate excitation (∼100 mJ/cm²) and a lifetime about 2 ps at high excitation (>160 mJ/cm²). The difference in the lifetime can be attributed to different gain mechanisms related to excitonic interaction and electron-hole plasma, respectively.     

垂直氧化锌纳米线中的激射现象

通过水热的方法以退火0.5 h的ZnO薄膜作为籽晶,得到垂直的ZnO纳米线.在X射线衍射谱中,除了Si的(400)衍射峰以外,只观察到了ZnO的(002)衍射峰.室温光致发光谱中出现了强的紫外发射峰,同时也伴随着弱的缺陷相关的发射.这些数据表明垂直的ZnO纳米线序列有着较好的晶体质量.同时,通过光泵浦也观察到了ZnO纳...     

Optical processes in the formation of stimulated emission from ZnO nanowires

This paper studies power dependent photoluminescence spectra, the stimulated emission occurring at ultraviolet (UV) band instead of the green emission band of ZnO nanowires, which are prepared with a chemical reduction method. The dynamics of the UV emission and green emission is given to demonstrate the reason of stimulated emission occurring at UV band but not the green emission band under high excitation, which indicates that the slow decay rate of trap state makes it easy to be fully filled and saturated, while the fast decay rate of near-band-edge exciton state makes the UV emission dominate the radiative recombination under high excitation. The UV emission, as well as the corresponding stimulated emission, occurs in competition with the green deep-trap emission. In addition, when pump fluence further increases, the multiple lasing modes appear. The dependence of these lasing modes on the pump fluence is first discussed. This diagram should be helpful to understand and design the optical nanodevices of ZnO nanowires.     

Effect of Mn doping on the microstructures and photoluminescence properties of CBD derived ZnO nanorods

Mn-doped ZnO nanorods were synthesized from aqueous solutions of zinc nitrate hexahydrate, manganese nitrate and methenamine by the chemical solution deposition method (CBD). Their microstructures, morphologies and optical properties were studied in detail. X-ray diffraction (XRD) results illustrated that all the diffraction peaks can be indexed to ZnO with the hexagonal wurtzite structure. Scanning electron microscope (SEM) results showed that the average diameter of Mn-doped ZnO nanorods was larger than that of the undoped one. Photoluminescence (PL) spectra indicated that manganese doping suppressed the emission intensity and caused the blue shift of UV emission position compared with the undoped ZnO nanorods. In the Raman spectrum of Mn-doped ZnO nanorods, an additional mode at about 525 cm⁻¹ appeared which was significantly enhanced and broadened with the increase of Mn doping concentration.     

六角锥状ZnO纳米结构的生长机理、结构及光学性能(英文)

利用醋酸锌[Zn(CH3COO)2·2H2O]和六次甲基四胺(C6H12N4)以一定比例配置成反应溶液,通过水热合成法制备了六角锥状ZnO纳米结构。同时,使用了扫描电子显微镜(SEM)、X射线衍射和选区电子衍射(SAED),对样品的形貌与结构进行了分析。结果表明,样品形貌成六角锥状结构,并且在[002]方向择优生长。通过对样品的光学性能测试,由PL光谱分析可知,样品在379nm处有一个较强的紫外发光峰,并且在可见光区域产生了一些较弱的可见光发射峰,表明制备的六角锥状ZnO纳米结构的晶体质量不是很好。除此之外,对六角锥状ZnO的生长机理也进行了讨论。     

Fabrication and strain investigation of ZnO nanorods on Si composing sol–gel and chemical bath deposition method

High density vertically aligned ZnO nanorods arrays were prepared on Si substrate by the simple and facile sol–gel and chemical bath deposition combination technology. ZnO nanorods, preferentially oriented along the c-axis, were of the hexagonal wurzite structure. The lattice constants of ZnO nanorods a was shrunken by about 0.004 nm, which can result in about 1.29% mismatch between ZnO nanorods and Si substrate. The Raman spectrum was also analyzed in detail, and the result indicates that the stress between ZnO nanorods and Si substrate was about 0.227 GPa, which can be ascribed to the stress relaxation effect of the ZnO nanorods. The room temperature photoluminescence (PL) measurement result has shown a main deep level emission. The forming mechanism for ZnO nanorods was further analyzed.     

Time-resolved photoluminescence on the stimulated emission in polycrystalline ZnO nanoparticles

The detailed room temperature stimulated emission including its optical characteristics from ZnO nanoparticles, which were prepared by a homogenous precipitation method, has been investigated by the time-resolved spectroscopy. The light emission originates from a free exciton recombination at a lower excitation level; the amplified spontaneous emission appears at a moderate excitation level, in which the threshold excitation intensity is 0.65 GW cm⁻². The resonant stimulated emission was observed in ZnO nanoparticles at a higher excitation intensity. Also, the emission lifetime is drastically reduced. Compared to the fluorescence decay curves, the time-resolved spectrum of the stimulated emission suggests the Gaussian-like decay time with only a few of picoseconds. The dynamic processes of lasing behavior and the characteristics of lasing emission in ZnO nanoparticles could provide the information on the crystal quality, the exciton and the lasing action in the particles.     

五边形截面的Ag纳米线局域表面等离子体共振模式

五边形截面的单晶Ag纳米线对ZnO量子点荧光具有增强的现象. 为解释这一现象, 利用时域有限差分法对五边形截面的Ag纳米线的局域表面等离子体共振模式进行了理论模拟. 结果表明, 五边形截面的Ag纳米线在紫外区域存在两个消光峰, 分别由Ag纳米线的横向偶极共振(340 nm)和四极共振(375 nm)引起; 这两个消光峰与ZnO量子点荧光增强峰相一致, 而且随着Ag纳米线的半径增大而红移; 消光峰对应的共振模式取决于Ag纳米线的截面形状; 根据Ag纳米线电场增强倍数与激发光波长变化关系曲线可知, 最大增强电场位于五边形截面的顶点处, 而边线处电场增强较小. 理论模拟的结果较好地解释了Ag纳米线/ZnO量子点体系的荧光增强现象, 也为Ag纳米线在提高半导体材料发光效率、生物探测等方面的应用提供有益的参考.     

ZnO纳米柱无序介质中泵浦面积对局域模发射的影响

基于ZnO纳米柱制备及发光实验,建立了ZnO纳米柱的位置和大小都是无序的二维介质结构模型.通过构建增益模型,用时域有限差分法数值模拟了无序介质中频谱特性以及ZnO增益频谱范围内的某一个共振峰对应的波源在无序介质中的光场分布情况,发现了局域模的存在.分四种情况讨论了此局域模的受激辐射与泵浦面积的关系:改变泵浦功率,从左到...     

Ultraviolet lasing and field emission characteristics of ZnO nano-rods synthesized by nano-particle-assisted pulsed-laser ablation deposition

We describe the lasing and the field emission characteristics of ZnO nano-rod crystals synthesized by nano-particle-assisted pulsed-laser ablation deposition, where nano-particles formed in the gas phase by the condensation of the laser-ablated species are transported on to the substrate to form nanorods. The nano-rod crystals having a hexagonal shape with a pyramidal top were synthesized on a sapphire substrate by a single-step process. The nano-rod crystals act as an efficient ultraviolet emitter showing the stimulated emission under an optical excitation and also act as field emitters with a current density of 1 mA/cm² at an electric field strength of 16 V/μm. PACS 42.70.Hj; 85.45.Db; 81.05.Ea; 81.15.Fy     

ZnO纳米柱无序介质中泵浦面积对局域模发射的影响

基于ZnO纳米柱制备及发光实验,建立了ZnO纳米柱的位置和大小都是无序的二维介质结构模型.通过构建增益模型,用时域有限差分法数值模拟了无序介质中频谱特性以及ZnO增益频谱范围内的某一个共振峰对应的波源在无序介质中的光场分布情况,发现了局域模的存在.分四种情况讨论了此局域模的受激辐射与泵浦面积的关系:改变泵浦功率,从左到右依次增加两层ZnO纳米柱泵浦和单独泵浦一个局域区域;泵浦功率一定时,增加泵浦局域区域和非局域区域中ZnO纳米柱个数.结果表明:存在一个临界泵浦功率,当泵浦功率小于临界泵浦功率时,无论泵浦面积多大都不能激发局域模;当泵浦功率大于临界泵浦功率时,对于不同的泵浦功率,局域模被激发所需的临界泵浦面积不同;随着泵浦功率的增加,当泵浦面积一定时,光场相对强度呈递增趋势,当泵浦功率超过临界功率时,光场相对强度急剧上升.     

Aerosol-based coherent random laser

We demonstrate coherent random lasing from an aerosol of dye-doped microdroplets in air. The aerosol is in the form of a linear array of polydisperse, arbitrarily shaped, and randomly spaced microdroplets with average dimensions of about 30 μm. Upon optical excitation, ultranarrow lasing modes were observed in the emission along the axis of the linear array, while the transverse emission exhibited intrascatterer resonance peaks. Direct spatiospectral imaging and lasing threshold studies confirmed the origin of the lasing peaks to be from spatial modes that extended over the array of the polydisperse microdroplets.     

A template-free sol-gel technique for controlled growth of ZnO nanorod arrays

The growth of ZnO nanorod arrays via a template-free sol-gel process was investigated. The nanorod is single-crystalline wurtzite structure with [0 0 0 1] growth direction determined by the transmission electron microscope. The aligned ZnO arrays were obtained directly on the glass substrates by adjusting the temperatures and the withdrawal speeds, without seed-layer or template assistant. A thicker oriented ZnO nanorod arrays was obtained at proper experimental conditions by adding dip-coating layers. Room temperature photoluminescence spectrum exhibits an intensive UV emission with a weak broad green emission as well as a blue double-peak emission located at 451 and 468 nm, respectively. Further investigation results show that the difference in the alignment of nanorods ascribes to the different orientations of the nanoparticles-packed film formed prior to nanorods on the substrate. Well ordered ZnO nanorods are formed from this film with good c-axis orientation. Our study is expected to pave a way for direct growth of oriented nanorods by low-cost solution approaches.     

氧化锌纳米棒场发射性能研究

采用简单物理气相沉积法制备出取向和非取向的氧化锌纳米棒，他们的场致电子发射性能测量结果表明，ZnO纳米棒具有较好的场发射性能，但是高度取向的ZnO纳米棒阵列并不利于获得高的场致电子发射电流密度.这可能是由于高密度ZnO纳米棒之间具有较高的屏蔽效应，降低了ZnO纳米棒阵列的场放大因子，从而影响了其场发射性能.相反，非取向ZnO纳米棒由于相互之间的屏蔽效应比较弱，而且表面存在容易成为发射中心的微小突起，表现出较好的场发射效果.这些结果不仅有助于加深我们对准一维纳米材料场致电子发射性能的理解，也为未来场发射电子器件的实际应用提供了可靠的依据. 关键词： 氧化锌 场发射 非取向     

Studies on structural and magnetic properties of Co-doped pyramidal ZnO nanorods synthesized by solution growth technique

Large-area arrays of highly oriented Co-doped ZnO nanorods with pyramidal hexagonal structure are grown on silica substrates by wet chemical decomposition of zinc–amino complex in an aqueous medium. In case of undoped ZnO with an equi-molar ratio of Zn²⁺/hexamethylenetetramine (HMT), highly crystalline nanorods were obtained, whereas for Co-doped ZnO, good quality nanorods were formed at a higher Zn²⁺/HMT molar ratio of 4:1. Scanning electron microscope (SEM) studies show the growth of hexagonal-shaped nanorods in a direction nearly perpendicular to the substrate surface with a tip size of ～50 nm and aspect ratio around 10. The XRD studies show the formation of hexagonal phase pure ZnO with c-axis preferred orientation. The doping of Co ions in ZnO nanorods was confirmed by observation of absorption bands at 658, 617 and 566 nm in the UV–vis spectra of the samples. The optical studies also suggest Co ions to be present both in +2 and +3 oxidation states. From the photoluminescence studies, a defect-related emission is observed in an undoped sample of ZnO at 567 nm. This emission is significantly quenched in Co-doped ZnO samples. Further, the Co-doped nanorods have been found to show ferromagnetic behavior at room temperature from vibrating sample magnetometer (VSM) studies.     

Influence of Sb on a controlled-growth of aligned ZnO nanowires in nanoparticle-assisted pulsed-laser deposition

Single-crystalline ZnO nanowires on a sapphire substrate have been synthesized by a nanoparticle-assisted pulsed-laser deposition (NAPLD) using a pure and Sb₂O₃ doped ZnO target. Low density and vertically well-aligned ZnO nanowires were grown on hexagonal cone-shape ZnO cores by introduction of a ZnO buffer layer. More than 90% of the ZnO cores of the Sb-induced ZnO nanowires are formed in the same size of 400 nm. The ZnO nanowires consist of single-crystalline wurtzite ZnO crystal and grow along [0001] direction. The room-temperature photoluminescence spectrum exhibited a strong ultraviolet emission at around 380 nm and a relatively low broad band emission in the visible region, indicating a low concentration of structural defect in the nanowires. Sb can be used as one of the effective additives to control the morphology and alignment of ZnO nanowires synthesized by NAPLD.     

氧化锌叶片状纳米晶的结构和光谱特性

熔盐法对sol-gel法生成的前驱物处理合成新颖的叶片状的氧化锌纳米结构,TEM照片显示其长度300-500nm,宽度为50-80nm,两头尖端约呈25°夹角,形状基本沿中轴呈中心对称。其生长过程进行了研究:弯曲了的ZnO纳米棒闭合形成框架结构,框架内沿中轴方向并排生长的ZnO纳米线填满框架内的空隙形成叶片状的氧化锌纳米结构。Raman谱测量发现该结构是晶化的六角相氧化锌。对叶片状的氧化锌的声子限制效应进行了研究,并与纳米颗粒氧化锌予以比较。435cm-1的E2峰的Fano不对称具有正的Fano耦合系数。发现在585nm处出现光致发光峰,归于ZnO纳米结构中氧缺陷的作用。