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.     

反饱和特性化合物锌四苯并卟吩巴豆酸苯氧树脂的光吸收谱测定

报道一种新型的有机材料锌—四苯并叶吩—巴豆酸—苯氧树脂(缩写为Zntbp—CA—PhR)体系薄膜样品的吸收谱的测定，及其主要吸收谱带在激光作用下的变化情况及动力学过程。实验观察到此种材料显著的饱和及反饱和吸收现象，并观察到它的再反饱和过程，定性分析了变化过程中的物理机制。这种特征在可见光波段一个较宽的区域内都会出现。所获结果为此种有机材料在光谱域信息存储和光学限制等方面的应用提供了理论和实验依据。     

Thermally induced nonlinear optical response and optical power limiting of acid blue 40 dye

We report the investigations of thermally induced third-order nonlinear optical and optical limiting characterizations for various concentrations of acid blue 40 dye in N,N-Dimethyl Formamide, studied by employing z-scan technique under cw He–Ne laser irradiation at 633 nm wavelength. The samples exhibited nonlinear absorption and nonlinear refraction under the experimental conditions. For lower concentration, the samples display both saturable absorption (SA) and reverse saturable absorption (RSA); whereas with increase in concentration, RSA behaviour prevails. The estimated values of the effective coefficients of nonlinear absorption β_eff, nonlinear refraction n₂ and third-order nonlinear susceptibility χ⁽³⁾ were found to be of the order of 10^?2 cm/W, 10^?4 esu and 10^?6 esu respectively. Multiple diffraction rings were observed when the samples were exposed to laser beam due to refractive index change and thermal lensing. The effect of concentration and the laser intensity on the self-diffraction ring patterns was studied experimentally. The acid blue 40 dye also exhibited strong optical limiting properties under cw excitation and reverse saturable absorption is found to be the dominant nonlinear optical process leading to the observed nonlinear behaviour.     

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.     

Rapid synthesize of gold nanoparticles by microwave irradiation method and its application as an optical limiting material

We present rapid synthesis of gold nanoparticles by microwave irradiation method. Sample with average particle size 7.7 nm is obtained from TEM. Linear and nonlinear optical studies of the prepared samples are discussed. Reverse saturable absorption (RSA) at longitudinal surface plasmon resonance (SPR) in gold nanoparticles (Au NPs) have been observed using Z-scan and transient absorption techniques with 532 nm laser pulses. Such RSA behavior makes Au NPs an ideal candidate for optical limiting applications.     

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.     

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.     

EXCITED-STATE NONLINEAR ABSORPTION AND ITS APPLICATION IN PHOTONIC TECHNOLOGY

The main achievements in our research on the physical phenomena of the excited-state nonlinear absorption in a molecular system and its applications in photonic technology are described. In the first part of this paper, some energy-level models and rate-equations are used to explain various mechanisms of the excited-state nonlinear absorption under differ-ent conditions, such as reverse saturable absorption caused by the triplet and/or the singlet excited-state absorption; saturable absorption due to the first and/or the second singlet excited-state absorption; and the excited-state nonlinear absorption induced by two-photon absorption. The experimental results for metal-organic and C₆₀ materials irradiated by ps and ns laser pulses are consistent with the simulated curves of the transmittance versus flu-ences. In the second part, the applications of excited-state nonlinear absorption in photonic techniques including optical bistability, optical switching, optical limiting, optical modula-tion, optical logic and optical storage are introduced. The working principles of the photonic devices based on the excited-state nonlinear absorption are presented. The experimental characteristic curves are found in good agreement with the theoretical simulations for these devices.     

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。     

Third-Order Nonlinear Optical Response near the Plasmon Resonance Band of Cu_(2-x)Se Nanocrystals

The third-order nonlinear optical properties of water-soluble Cu_(2-x)Se nanocrystals are studied in the near infrared range of 700-980 nm using a femtosecond pulsed laser by the Z-scan technique. It is observed that the nonlinear optical response of Cu_(2-x)Se nanocrystals is sensitively dependent on the excitation wavelength and exhibits the enhanced nonlinearity compared with other selenides such as ZnSe and CdSe. The W-shaped Z-scan trace, a mixture of the reversed saturated absorption and saturated absorption, is observed near the plasmon resonance band of Cu_(2-x)Se nanocrystals, which is attributed to the state-filling of free carriers generated by copper vacancies(self-doping effect) of Cu_(2-x)Se nanocrystals as well as the hot carrier thermal effect upon intense femtosecond laser excitation. The large nonlinear optical response and tunable plasmonic band make Cu_(2-x)Se nanocrystals promising materials for applications in ultra-fast all-optical switching devices as well as nonlinear nanosensors.     

Nonlinear optical switching and all-figures of merit in Bi2S3-xSex/PMMA nanocomposite films investigated by Z scan under visible CW laser

Bi2S3-xSex/poly(methyl methacrylate)(PMMA)nanocomposite films were prepared using microwave assisted synthesis with different compositions of x.Crystal structure,surface morphology,and optical properties were investigated to characterize the prepared nanocomposite films.The crystallinity and optical band gap of the prepared Bi2S3-xSex/PMMA were affected by x.The prepared samples showed a blue shift in the absorption edge.The laser power dependent nonlinear refraction and absorption of Bi2S3-xSex/PMMA nanocomposite films were investigated by using the Z-scan technique.The optical nonlinearity of the nanocomposite films exhibited switchover from negative nonlinear refraction to positive nonlinear refraction to negative nonlinear refraction effects,and from saturable absorption to reverse saturable absorption to saturable absorption with an increase and decrease in the composition.An interesting all-optical figure of merit was reported to assess the nanocomposite films for a practical device.It was calculated that the device all-figures of merit were based on the nonlinear response,which is important for the all-optical switching device.The results demonstrate that the optimized all-optical figures of merit can be achieved by adjusting the composition and input laser power,which can be used for the design of different all-photonic devices,and the results of nonlinear switching behavior can open new possibilities for using the nanocomposite films in laser Q-switching and mode-locking.     

Ultrafast Saturable Absorption of Core/Shell Colloidal Quantum Dots

Ultrafast saturable absorption (SA) materials that are capable of blocking the optical absorption under strong excitation have extensive applications in photonic devices. This work presents core/shell colloidal quantum dots (CQDs) which have the quantized energy levels, excellent band gap tunability, and possess significant SA performance. When the band gap is close to the pump pulse energy, the CQDs show significant resonant SA response. At the same excitation conditions, the core/shell CQDs dispersions show better SA response than graphene dispersions, and comparable to the recently reported molybdenum disulfide. The carrier dynamics of the SA of the CQDs is analyzed systematically. The research has also found that the two‐photon absorption of the CQDs show nearly cubic power law of the band gap, while the SA performance keeps almost the same in the nonresonant regime. Further, superior passive Q‐switched laser behavior is observed using the CQDs as a saturable absorber. The results directly reveal the physical processes of this basic problem and broaden the applications of CQDs in photonic devices.     

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.     

The theory and experiment of solute migration caused by excited state absorptions

Nonsymmetrical transition from reverse-saturable absorption (RSA) to saturable absorption (SA) caused by excited state absorption induced mass transport of the CuPcTs dissolved in dimethyl sulfoxide is observed in an open aperture Z-scan experiment with a 21-ps laser pulse. The nonsymmetrical transition from RSA to SA is ascribed neither to saturation of excited state absorption nor to thermal induced mass transport, the so-called Soret effect. In our consideration, strong nonlinear absorption causes the rapid accumulation of the non-uniform kinetic energy of the solute molecules. The non-uniform kinetic field in turn causes the migration of the solute molecules. Additionally, an energy-gradient-induced mass transport theory is presented to interpret the experimental results, and the theoretical calculations are also taken to fit our experimental results.     

被动光学限幅器的机制与研究进展

被动光学限幅器是利用介质的非线性光学性质实现对光的强度进行控制的器件，它在科研，军事和民用方面都具有广泛的应用，文章讨论了被动光学限幅器的反饱和吸收，双光子吸收，自由载流子吸收，非线性折射，光致散射和光折变机制，每种机制在光限幅器应用中的有效性及局限性，介绍了国内外研究状况及自己的工作；指出了今后被动光学限幅器研究的发展方向。     

Study of absorption spectrum and dynamics evaluation of the indocyanine‐green first singlet excited state

Excited state absorption and excited state dynamics of indocyanine‐green (ICG) dissolved in dymethyl sulfoxide were measured using white‐light continuum Z‐scan (WLCZScan) and white‐light continuum pump–probe (WLCPP) techniques. The excited state absorption spectrum, obtained through Z‐scan measurements, revealed saturable absorption (SA) for wavelengths longer than 630 nm, while reverse saturable absorption (RSA) appeared, as indicated by a band at approximately 570 nm. Both processes were modeled by a three‐energy‐level diagram, from which the excited state cross‐section values were determined. SA and RSA were also observed in pump–probe experiments, with a recovery time in the hundreds of picoseconds time scale due to the long lifetime of the first excited state of ICG. Such results contribute to the understanding of ICG optical properties, allowing application in photonics and medicine. Copyright © 2010 John Wiley & Sons, Ltd.     

掺Er3+玻璃的光限幅特性研究

利用波长为532 nm的皮秒脉冲激光,研究了掺Er3 玻璃的光限幅特性和反饱和吸收.当入射功率不断增加且超过一定阈值时,透射功率不再随着入射功率快速增大,而是逐渐趋向于较稳定状态,从而实现了对强激光的光限幅效应.进一步利用布居速率方程讨论了其机制并给出了激发态的吸收截面,结果表明激发态吸收是其主要的光限幅机理.     

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.     

碳纳米管/二硒化钼有机玻璃的非线性吸收、非线性散射和光限幅特性

MoSe₂的禁带宽度较窄（1.1–1.5 eV）,且具有可调谐的激子光电效应,这样使其在光致发光、光电晶体管、太阳能电池和光学非线性等方面具有潜在的应用价值.然而,纯的MoSe₂的光生电子空穴复合率较高,限制了其在某些光学领域中的应用.通过设计MoSe₂的复合材料,可以降低材料的光生电子空穴复合率,从而扩展其应用领域.首先,通过热溶剂法合成CNT/MoSe₂复合材料;然后,通过浇铸法将其分散在甲基丙烯酸甲酯（MMA）中制备成有机玻璃,其中MMA会聚合成聚甲基丙烯酸甲酯（PMMA）,并利用改进的Z-扫描技术首次对CNT/MoSe₂/PMMA有机玻璃的非线性吸收、非线性散射和光限幅特性进行了研究.研究表明,随着输入能量的变化,通过调节输入能量,CNT/MoSe₂/PMMA有机玻璃表现出饱和吸收（SA）和从SA到反饱和吸收的转变.结合材料特性及应用条件要求,可以得到CNT/MoSe₂/PMMA有机玻璃在光学设备,如光学限制器和锁模/调Q激光器等方向具有较好的应用前景.     

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.