Picosecond nonlinear optical properties of cuprous oxide with different nano-morphologies

Cuprous oxide nanoclusters, microcubes and microparticles were successfully synthesized by a simple co-precipitation method. Phase purity and crystallinity of the samples were studied by using X-ray powder diffraction. Transmission electron microscopy (TEM) images show different morphologies like nanoclusters, microcubes and microparticles. For linear and nonlinear optical measurements, the as-synthesized Cu₂O with different morphologies were dispersed in isopropanol solution. The absorption spectrum recorded in the visible regions shows peaks that depend on the morphology of the particles and the peak shifts towards red region as one goes from nanoclusters to microparticles. Simple open-aperture Z-scan technique is used to measure nonlinear optical properties of cuprous oxide at 532 nm, 30 ps excitation at 10 Hz repetition rate. Cuprous oxide nanoclusters show reverse saturable absorption (RSA) behaviour, the microcubes and microparticles at a similar concentration exhibit saturable absorption (SA) type of behaviour at lower peak intensities and exhibit RSA within SA at higher peak intensities. The results show that the transition from SA to RSA can be ascribed to the two-photon absorption (TPA) process.     

Effect of marine derived deoxyribonucleic acid on nonlinear optical properties of PicoGreen dye

We have investigated the effect of DNA on nonlinear absorption of PicoGreen dye using single beam open aperture Z-scan technique in nanosecond regime. We observed reverse saturable absorption at 532 nm for PicoGreen without DNA. In the presence of DNA, the sample begins to behave like saturable absorbers and this effect increased as the concentration of DNA was increased. The dye-intercalated DNA showed SA characteristics near the focus but exhibited RSA characteristics at the focus. Theoretical analysis has been performed using a two-photon absorption model based on nonlinear absorption coefficient and saturation intensity. Such tailoring of optical nonlinear absorption in PicoGreen makes it a potential candidate for photonic application.     

Gold Nanocages as Effective Photothermal Transducers in Killing Highly Tumorigenic Cancer Cells

Numerous gold nanostructures have the potential for photothermal therapy in cancers. Here, gold nanocages and gold nanoshells are synthesized, the sizes of which are fine‐tuned for a response at 750 nm wavelength. Their photothermal therapeutic efficiency is compared at gold concentration of 100 lg mL^?1 using a near‐infrared laser (750 nm). The biocompatibility for varying concentrations of gold (1 to 100 lg mL^?1) is performed in a normal cell line and laser‐mediated cell cytotoxicity for varying time intervals (7.5 and 10 min) is carried out in breast cancer cells. This study shows that when analyzed under similar conditions, the gold nanocages show better biocompatibility and are more efficient in near‐infrared absorption and photothermal conversion in comparison with conventional gold nanoshells. When subjected to photothermal laser ablation of breast cancer cell line for 7.5 min and 10 min, the nanocages are able to induce 62.92 ± 3.25% and 96.41 ± 3.04% reduction in cell viability, respectively, in comparison to nanoshells, in which a 43.35 ± 1.91% and 79.89 ± 4.74% reduction in cell viability is observed. The current study shows that the gold nanocages can outperform gold nanoshells and effectively kill cancer cells without any significant cytotoxic effect on normal cells.     

GaN晶体在飞秒紫外波段激发下的可变非线性吸收效应和光动力学过程研究

采用Z扫描和泵浦-探测技术研究了GaN薄膜在370 nm时的非线性光学效应和非线性光动力学过程。首先,基于GaN薄膜的透射光谱,结合线性光学理论分析得到了其在370 nm的线性折射率n₀、线性吸收系数α₀、光学带隙E_g等线性光学性质。采用飞秒激光Z扫描技术,得到了不同光强激发下的Z扫描实验响应结果,结合非线性光学理论提取出GaN薄膜可变的光学非线性吸收效应。在激发光子能量接近GaN带隙情况下,低光强时材料表现为饱和吸收而高光强时为反饱和吸收,这是因为低光强下单光子吸收占主导而高光强下以单光子感应自由载流子吸收为主。闭孔Z扫描测量得到了GaN薄膜的三阶非线性折射系数为n₂=-(1.0±0.1)×10-3 cm2·GW-1,它几乎比传统非线性介质的高出一个数量级。为了探究上述非线性过程的动力学弛豫时间以及进一步探究GaN薄膜非线性光动力学过程的深层物理机制,采用了交叉偏振飞秒退相泵浦探测技术观察GaN薄膜的光激发载流子动力学弛豫过程。实验结果表明,在低光强下,饱和吸收效应来源于瞬态单光子吸收,高光强下单光子感应自由载流子吸收为非瞬态光动力学过程,其自由载流子弛豫时间约为17 ps。该工作将为GaN薄膜在紫外非线性纳米器件应用以及GaN薄膜非线性过程的机制分析理解提供新的思路。     

Effects of solvent on nonlinear absorption properties of tetraphenylporphyrin compounds in the nanosecond regime

The nonlinear absorption properties of tetraphenylporphyrins (TPP) in different solvents and excitation intensities are investigated with nanosecond pulses by the Z-scan technique. The nonlinear absorption behaviour observed presents a distinct difference between in solvent mixtures and in pure solvents. A crossover from reverse saturable absorption (RSA) to saturable absorption (SA) and then again to RSA is observed with the increases of excitation intensity in chloroform and pyridine mixed solvents. However, porphyrin molecules in pure solvents show good RSA behaviour under the studied intensity range, no saturation absorption is observed with nanosecond excitation. Excited state absorption parameters and two-photon absorption coefficients are obtained by theoretical fit using rate equations for population densities in a seven-level energy scheme.     

Gold nanocages as contrast agents for spectroscopic optical coherence tomography

We describe gold nanocages as a new class of potential contrast agent for spectroscopic optical coherence tomography (OCT). Monodispersed gold nanocages of an approximately 35 nm edge length exhibit strong optical resonance, with the peak wavelength tunable in the near-infrared range. We characterized the optical properties of the nanocage by using OCT experiments along with numerical calculations, revealing an absorption cross section approximately 5 orders of magnitude larger than conventional dyes. Experiments with tissue phantoms demonstrated that the nanocages provide enhanced contrast for spectroscopic as well as conventional intensity-based OCT imaging.     

Z-scan analytical theory for material with saturable absorption and two-photon absorption

By using the Adomian decomposition method, we present the transmitted optical intensity of a nonlinear medium with the concurrence of saturable absorption (SA) and two-photon absorption (TPA) processes. We obtain the analytical expression of the open-aperture Z-scan and investigate the interplay between SA and TPA in the Z-scan trace. Through Z-scan measurements at different levels of laser intensities, both the saturable intensity and TPA coefficient could be obtained quickly yet unambiguously.     

基于铋可饱和吸收体的超快激光产生

采用磁控溅射沉积法在微纳光纤表面上镀一层纳米级厚度的铋薄膜,制备了一种微纳光纤-铋膜结构的可饱和吸收体.在1.5μm处的非线性光调制深度为14%.将其应用到掺铒光纤激光器中,在1.5μm波段获得稳定的超快脉冲激光产生,脉宽为357 fs,输出功率为45.4 mW,单脉冲能量为2.39 nJ,信噪比为84 dB.实验结果表明,利用磁控溅射法可制备出大调制深度的可饱和吸收体,为获得高能量超短脉冲激光输出提供新方案.     

Observation of simultaneous reverse saturation absorption and saturation absorption in silver nanoparticles incorporated into europium oxide thin film

In this work, nano silver clusters incorporated into europium oxide thin films at a level of 3.8% and 12.5% have been prepared by a vacuum evaporation method on glass and silicon substrates. Samples were investigated by X-ray fluorescence, X-ray diffraction, and linear and nonlinear optical absorption methods. The X-ray diffraction reveals that the Eu oxide of these samples remains amorphous after pre-annealing at 400 °C. The linear optical absorption of the samples shows surface plasmon resonance (SPR) phenomena, which varies with the Ag content of the samples. The optical nonlinear absorption properties of the prepared films were investigated using an open Z-scan technique with cw laser at wavelengths 476 nm and 514 nm. A changeover from reverse saturation absorption (RSA) to saturation absorption (SA) was observed. RSA is attributed to interband transition via two photon absorption. SA is attributed to plasmon bleach.     

Diffraction patterns and nonlinear optical properties of gold nanoparticles

Stable gold nanoparticles have been prepared by using soluble starch as both the reducing and stabilizing agents; this reaction was carried out at 40 °C for 5 h. The obtained gold nanoparticles were characterized by UV–Vis absorption spectroscopy, transmission electron microscopy (TEM) and z-scan technique. The size of these nanoparticles was found to be in the range of 12–22 nm as analyzed using transmission electron micrographs. The optical properties of gold nanoparticles have been measured showing the surface plasmon resonance. The second-order nonlinear optical (NLO) properties were investigated by using a continuous-wave (CW) He–Ne laser beam with a wavelength of 632.8 nm at three different incident intensities by means of single beam techniques. The nonlinear refractive indices of gold nanoparticles were obtained from close aperture z-scan in order of 10^?7 cm²/W. Then, they were compared with diffraction patterns observed in far-field. The nonlinear absorption of these nanoparticles was obtained from open aperture z-scan technique. The values of nonlinear absorption coefficient are obtained in order of 10^?1 cm/W.     

Nonlinear susceptibility of a metal-dielectric nanocomposite caused by induced dipole-dipole forces between particles

The optical coefficients of a nonlinearity for a macroscopic ensemble of aggregates of metal nanoparticles that is caused by deformation of the spatial structure of clusters in a strong light field are calculated for the first time. For a continuous medium that consists of a nonabsorbing dielectric containing aggregated silver nanoparticles that do not possess an intrinsic optical nonlinearity, coefficients of nonlinear absorption are obtained in relation to the intensity and frequency of incident light. It is shown that, at intensities of up to a few megawatts per square centimeter, the addition to the absorption of a nanocomposite to be modeled is adequately described by a third-order nonlinearity. The magnitude and sign of the nonlinear absorption coefficient agree well with the previously obtained experimental data for aggregated silver and gold colloids under nanosecond excitation.     

CdSe/ZnS核-壳结构量子点的非线性光学吸收

利用开孔Z扫描技术研究了吸收峰分别为553 nm和503 nm的两种尺寸CdSe/ZnS核-壳结构量子点溶液的非线性吸收性质.对于532 nm,6 ns激光脉冲,两种材料均表现出饱和吸收向反饱和吸收转化的现象.数值模拟结果表明：当吸收峰波长大于激光波长时,饱和吸收过程由快、慢两种机制组成,分别对应基态载流子被激发至不同的激发态,而强光下的反饱和吸收与快过程相关;当吸收峰波长小于激光波长时,饱和吸收主要由快过程机制引起,强光下的反饱和吸收源自激发态吸收和双光子吸收.我们的研究结果表明半导体量子点是研制光开关和光限制器件的理想候选材料.     

All-optical ultrafast logic gates based on saturable to reverse saturable absorption transition in CuPc-doped PMMA thin films

A detailed theoretical analysis of femtosecond transition from saturable (SA) to reverse saturable absorption (RSA) has been carried out in Copper-Phthalocyanine (CuPc)-doped polymethylmethacrylate (PMMA) thin films. The transition due to fifth-order effect of excited-state absorption induced two-photon process has been optimized with respect to intensity, concentration and nonlinear coefficients to design various all-optical logic gates, namely, OR and AND at lower intensities (SA region), XOR at the transition intensity, and the universal NAND and NOR at higher intensities (RSA region). The advantages of ultrafast operation, simplicity, tunability, high contrast, stability of CuPc-doped PMMA thin film, and the possibility to control and realize various logic operations in the same film at the same wavelength by only controlling the pulse intensity, instead of a pump-probe configuration, make them attractive for practical implementation.     

不同表面结构的金纳米粒子荧光性质.

"研究了具有不同表面结构的金纳米粒子：裸金纳米粒子、三苯基膦修饰的金纳米粒子、巯基丙酸表面取代的金纳米粒子的荧光性质,及其对CdSe纳米粒子的荧光猝灭作用．发现不同的金纳米粒子荧光信号受粒子表面一价金离子与配体分子之间相互作用的影响,其荧光强度对其表面分子具有强烈的敏感性;具有不同表面结构的金纳米粒子对CdSe纳米粒子的荧光猝灭作用不同,与其吸收光谱和CdSe纳米粒子发射光谱的重叠程度相关."     

Observation of nonlinear saturable and reverse-saturable absorption in silver nanowires and their silica gel glass composite

Silver nanowires (Ag NWs) and their silica gel glass composite were produced. Their nonlinear optical (NLO) properties, mainly saturable absorption (SA) and reverse-saturable absorption (RSA), were investigated at 532 and 1064 nm, using the open aperture z-scan technique and a nanosecond-pulsed laser. We found that Ag NWs demonstrate rather different NLO behaviors in liquid and solid-state matrices. The Ag NWs suspension exhibited only RSA, whereas a transformation from SA to RSA occurred in the silica gel glass composite. The underlying mechanism was proposed from the viewpoint of different environments and electronic dynamics of Ag NWs in the liquid and solid-state matrices.     

The third order nonlinear optical characteristics of amorphous vanadium oxide thin film

We studied the nonlinear absorptive characteristics (saturation intensity threshold and effective nonlinear absorption coefficients) and nonlinear refraction in a 50-nm-thick VO _x thin amorphous film prepared by pulsed DC magnetron reactive sputtering. The absorptive and refractive nonlinearities were investigated by pump–probe and Z-scan techniques. The closed-aperture Z-scan results reveal self-defocussing characteristics of the amorphous VO _x thin film for both nanosecond and picosecond pulse durations. Experimental results show that a phase transition does not occur in the range of intensities used for the experiments and the investigated sample can be treated as an amorphous semiconductor structure. The open-aperture Z-scan curves with nanosecond pulses exhibit saturable absorption for all input intensities. On the other hand, the open-aperture Z-scan curves with picosecond pulses exhibit nonlinear absorption/saturable absorption for low/high input intensities, respectively. Saturation intensity thresholds were found to be 15.3 MW/cm² for 4-ns pulse duration and 586 MW/cm² for 65-ps pulse duration.     

基于虚拟仪器的高精度Z扫描实验系统设计

设计了一个表征样品非线性特性的基于虚拟仪器的z扫描实验系统。利用Labview控制数字示波器TDS3012采集两路光强信号，并结合对微位移平台的控制实现Z扫描。以Nd：YAG飞秒放大器产生的800nm的飞秒激光作为探测光，经透镜聚焦后通过薄介质样品；用数字示波器测量样品在透镜焦点附近的透射光强，经过数据处理得到样品的非线性折射率和非线性吸收系数。利用该实验系统，对标准非线性吸收样品Rhodamine 6B进行了测量，计算得到其双光子吸收截面为σ^2=6．8GM（GM：10^-50cm4s photon^-1 molecule^-1），该结果与其他文献利用不同测量方法得到的结果接近，证明该实验系统的测量结果是正确的，可满足非线性测量的精度要求。     

基于金纳米笼的1106 nm被动调Q Nd:GAGG激光器

成功制备了金纳米笼溶液并将其作为饱和吸收体,实现了中心波长为1106 nm的Nd:GAGG激光器的调Q运转。在输出镜透过率为3%的激光器中,在泵浦功率6.70 W下获得的最大平均输出功率为98 mW,此时对应的脉冲重复率为206 kHz,最短脉冲宽度为436 ns;在输出镜透过率为7%的激光器中,当泵浦功率为7.69 W时,得到的最大平均输出功率为121 mW,最短脉冲宽度为370 ns,对应的脉冲重复率为170 kHz。实验结果证明了金纳米笼在近红外波段激光器中用作饱和吸收体的巨大潜力。     

Controllable Preparation of Hierarchical ZnO Nanocages and its Oxygen Vacancy through the Nanoscale Kirkendall Process

The synthesis of ZnO with tailorable shapes and point defects is important for its potential applications. Here, a facile approach is demonstrated to prepare ZnO nanocages with controllable porous shell structures though sintering a Zn‐based cyanide‐bridged coordination polymer under different temperatures. The transformation of ZnCP microspheres into ZnO nanocages is based on two types of nanoscale Kirkendall effect, which are related to low temperature solid–solid interfacial oxidation and high temperature solid–gas interfacial reaction, respectively. At low temperature (around 300 °C) and before the ZnCP decomposition, the novel “hierarchical ZnO bigger nanocages embedded with smaller nanocages with 10 nm nanocrystals” can be generated. By contrast, when coming to the total decomposition of ZnCP at 800 °C, ZnO nanocages with significantly increased sizes and large cavities are generated, and large amounts of oxygen vacancies (V_O) are created at the same time, leading to the dramatic increased luminescence intensities of the UV peak due to V_O at 540 nm. Thus, the luminescence intensities versus defect concentration in the prepared ZnO nanocages can also be controlled by tuning the sintering temperatures.     

Modeling and identification on nonlinear saturable and reverse-saturable absorptions of gold nanorods using femtosecond Z-scan technique

An improved Z-scan analysis approach is proposed by establishing and solving the saturable absorption (SA) and reverse-SA (RSA) models, respectively. Near-infrared femtosecond Z-scans are carried out on the synthesized gold nanorods (NRs) possessing the average length of 46 nm using a femtosecond laser operated at the wavelength of 800 nm, which is close to the peak position of longitudinal surface plasmon resonance (SPR) (710 nm) of gold NRs. At lower input intensity of less than 400 GW/cm2 , the normalized transmission exhibits only SA phenomenon; however, when it exceeds 400 GW/cm2 , both SA and RSA are observed. By using the presented Z-scan modeling and theory, the three-photon absorption (3PA) is identified in the material, and the 3PA cross-section is determined to be 1.58×1071 cm6s2 .