Excited state absorption of 1,3,3,1′,3′,3′-hexamethylindotricarbocyanine Iodide: A quantitative study by ultrafast absorption spectroscopy

A quantitative investigation of HITC dissolved in methanol has been made using the method of ultrafast absorption spectroscopy with a streak camera. Samples were excited by picosecond pulses of a mode-locked ruby laser. Analysis of time-resolved spectra yielded non-exponential decay kinetics consisting of a fast (τ variable) and a slow (τ=1.13±0.08 ns) component. The excited state absorption spectrum has its maximum at 493 nm and shoulders at 415 and 540 nm. The excited state absorption cross section was determined by simulataneous measurement of the bleaching of ground state absorption taking polarization of excitation and probe light and excited state absorption at the laser wavelength into account. A value of σ₁ (493 nm)=1.0·10^?16 cm² was found.     

Optical limiting properties of zinc phthalocyanines in solution and solid PMMA composite films

The nonlinear absorption and optical limiting (OL) performance of tetra- and octasubstituted zinc phthalocyanine complexes were described in solution and in the solid state using the open-aperture Z-scan technique. The measurements were performed using collimated 4 ns pulses generated from a frequency-doubled Nd:YAG laser at 532 nm wavelength. The polymeric films exhibit a much larger effective nonlinear absorption coefficient in comparison with solution. However, the parameters of the ratio of the excited to ground state absorption cross section and energy-dependent saturation in solution are much better compared to properties in the polymeric film. In terms of the ratio of the excited to ground state absorption cross section, the peripherally substituted complexes show better OL performance than the non-peripherally substituted derivative.     

OPTICAL LIMITING EFFECT IN TWO PHTHALOCYANINES OBSERVED BY PICOSECOND PULSED LASER

Optical limiting (OL) properties of two phthalocyanines were investigated by using picosecond laser pulses at 532nm. The relative ratios k of the absorption cross section of the first singlet excited state to that of the ground state were approximately obtained by the analysis of the experimental results in which the reverse saturable absorption model of the three-energy-level scheme was employed. A significant comparison with fullerene C₆₀ was presented for OL. The OL mechanisms have been analysed in detail.     

Excited state refraction of C70/toluene studied by using 4f coherent imaging system with phase object

Dynamic nonlinearities of C₇₀/toluene solution are measured and analysed by an improved picosecond time-resolved pump-probe system based on a nonlinear imaging technique with phase object. The photophysical parameters are determined by the five-level model, which is adopted to interpret the experimental data. The change of refraction index per unit density of the excited state obtained by a numerically simulation is a critical factor to determine the nonlinear behaviour of C₇₀ in picosecond time regime.     

六能级分子系统非线性极化率的微观描述

本文从半经典密度矩阵理论出发,推出描述光与有机分子系统相互作用的非线性极化率、非线性折射率和非线性吸收系数的微观表达式,同时引入折射体积和吸收截面以描述布居于各能级单分子折射和吸收特性.     

GaAs在光通讯波段的超快非线性光学研究

采用Z-扫描和泵浦-探测技术,在光通讯波段对砷化镓(GaAs)单晶进行了非线性动力学以及非线性光学的实验研究.飞秒泵浦-探测实验结果表明,三阶非线性光学效应源于砷化镓单晶对飞秒激光的瞬态双光子吸收,而五阶非线性光学效应源于砷化镓单晶双光子吸收诱导的自由载流子吸收效应.通过Z扫描实验,得到了关于GaAs单晶所有的非线性光学参数,包括双光子吸收系数、三阶非线性折射系数、双光子吸收诱导的自由载流子吸收截面以及双光子吸收诱导的自由载流子折射截面.结果表明,砷化镓单晶在制造光限幅器件和光电探测器方面具有良好的发展前景.     

强非线性吸收下Z扫描衍射模型及实验研究

根据光的衍射理论,建立了非线性光学介质对高斯光束的开孔Z 扫描理论模型.数值计算表明,当相移比值Γ≤0.15,出射光功率随入射光功率的增加出现振荡衰减现象;当Γ>0.15,在输入光强低于某一个值时,输出随输入的增加而线性增加;当输入光强超过该值后,输出功率不再增加甚至趋于零.实验采用Nd∶YAG脉冲激光,在波长为532 nm,脉宽8 ns条件下,对含3.5%和7.0%碳纳米管的聚苯胺/碳纳米管复合体薄膜（PANI/MWCNT）的非线性吸收特性进行了研究.计算表明,该类化合物的激发态吸收截面积远大于其基态吸收截面积,具有很强的反饱和吸收.     

Effects of metallization and bromination on nonlinear optical properties of diphenylporphyrins

Nonlinear refraction and nonlinear absorption of diphenylporphyrins with bromination and metallization were studied by Z-scan technique in nanosecond and picosecond regimes. Results show that both metallization and bromination of diphenylporphyrins can cause the regular change of magnitude and sign of nonlinear absorption. The transition between saturable absorption and reverse saturable absorption happens as bromine increases and metal ion changes. The effect of bromination on nonlinear refraction is small, the change of nonlinear refraction is mainly attributed to the metallization. Influences of photophysical parameters on nonlinear absorption and nonlinear refraction have been elucidated using five-level models.     

The nonlinear optical response of a fluorine-containing azoic dye

The nonlinear optical nonlinearities of a fluorine-containing azoic dye in tetrahydrofuran have been investigated by using Z-scan technique with picosecond and nanosecond lasers. The experimental results reveal that the azoic dye has large optical nonlinearity under the excitations of picosecond and nanosecond 532 nm. At the picosecond 532 nm the solution presents negative nonlinear refraction due to the electronic effect, while the larger nonlinear refraction under nanosecond laser excitation is induced by thermal effect. Moreover, the different nonlinear absorption behavior under picosecond and nanosecond excitations is analyzed.     

Characterization of nonlinear optical parameters of polymethine dyes

We investigated nonlinear refraction, nonlinear absorption, and saturable absorption of polymethine dyes by the Z-scan technique (λ=1064 nm). The analysis of simultaneous appearance of several nonlinear optical processes in dye solutions excited by picosecond pulses was carried out. The saturable absorption was analyzed taking into account various models. Nonlinear refractive indices, nonlinear absorption coefficients, and saturation intensities of various polymethine dyes were measured. Received: 27 December 2002 / Revised version: 6 March 2003 / Published online: 5 May 2003 RID="*" ID="*"Corresponding author. Fax: +81-471/363-366, E-mail: r_ganeev@issp.u-tokyo.ac.jp RID="**" ID="**"Present address: The Institute for Solid State Physics, The Tokyo University, 5-1-5 Kashiwanoha, Kashiwa, Chiba 277-8581, Japan     

一种新型有机金属化合物纳秒时域饱和吸收特性研究

合成了一种新型有机金属配合物Cetyltrimethylammonium-bis(2-thioxo-1,3- dithiole- 4,5-dithiolato)-copper(简称CtCu)材料.采用单光束Z扫描测试技术,在波长为1 053 nm,脉宽为1 ns的条件下研究了该样品的三阶非线性光学性质.研究发现,该材料具有很强的饱和吸收特性,激发态的有效吸收截面为σeff＝1.10×10－19 cm2,与基态吸收截面的比值为1∶484.利用非线性透过率实验验证了材料的饱和吸收特性,并对其产生机理进行了分析.实验结果表明,该材料在近红外波段的激光脉冲压缩方面有潜在的应用前景.     

Excited State Absorption Study in Hematoporphyrin IX

We present the study of the excited state absorption of Hematoporphyrin IX dissolved in dimethyl sulfoxide. All measurements were carried out using open aperture Z-scan and white-light continuum pump-probe with picosecond pulses to avoid triplet excited state absorption. Without the latter contribution, the results obtained with both techniques show a transition to a high singlet excited state. The vibronic progression of the Q-band is observed due to photobleaching of the ground state. In addition, we show that the excited state presents reverse saturable absorption for most of the spectral range studied. A long relaxation component of the first singlet excited state was evidenced with the pump-probe experiment. This result is in agreement with fluorescence lifetime and fluorescence quantum yield measurements. In order to elucidate the origin of the nonlinear effects, we used a three-level energy diagram to describe the principal singlet-singlet transitions.     

Nonlinear atomic response to intense ultrashort x rays

The nonlinear absorption mechanisms of neon atoms to intense, femtosecond kilovolt x rays are investigated. The production of Ne(9+) is observed at x-ray frequencies below the Ne(8+), 1s(2) absorption edge and demonstrates a clear quadratic dependence on fluence. Theoretical analysis shows that the production is a combination of the two-photon ionization of Ne(8+) ground state and a high-order sequential process involving single-photon production and ionization of transient excited states on a time scale faster than the Auger decay. We find that the nonlinear direct two-photon ionization cross section is orders of magnitude higher than expected from previous calculations.     

反-4,4''-双(N,N-二丁胺基)二苯乙烯分子双光子吸收性质研究

对于实验室合成的反-4,4'-双(N,N-二丁胺基)二苯乙烯分子,实验测量了该分子的单光子和双光子荧光谱,然后从理论上研究了其单光子和双光子吸收特性.研究结果表明,在低能量范围内,分子的单光子吸收主要发生在分子的第一激发态,而分子的双光子吸收主要发生在分子的第二和第四激发态上.该分子在相应系列衍生物中具有最大的双光子吸收截面.分子的相关能对分子的激发态能量影响较大.我们给出了分子基态与电荷转移态的电荷转移过程,并从理论上定性解释了双光子聚合反应的聚合机理.     

The use of three-photon absorption for optical limiting of laser radiation

The results of a study of nonlinear refraction and nonlinear absorption at a wavelength of 532 nm in an LGO (Li₂Ge₂O₁₅) crystal by Z-scan methods are presented. It is shown that the nonlinear refraction is caused by self-focusing of the laser radiation, whereas the nonlinear absorption is three-photon in nature. The possibility of using an LGO crystal for producing the optical limiting of laser radiation of picosecond duration is demonstrated.     

Nonlinear optical characteristics of polymethine dyes

Nonlinear refraction, nonlinear absorption, and saturated absorption of a number of polymethine dyes are studied and their nonlinear optical parameters are measured by the Z-scan method (λ=1064 nm). Simultaneous occurrence of several nonlinear optical processes in the case of excitation of dye solutions by picosecond pulses is analyzed. Saturated absorption of dye solutions is considered in terms of different models.     

二苯乙烯衍生物分子双光子吸收截面：官能团对称性的影响

选取了具有不同对称性的二苯乙烯系列衍生物分子，在HF水平上，利用响应函数方法，研究了该系列分子的单光子和双光子特性. 研究结果表明，该系列分子具有较强的双光子特性. 在可见光范围内，反对称分子的最大双光子吸收态是第一激发态，而对称分子的最大双光子吸收出现在第四激发态. 相对于对称分子而言，反对称分子具有更大的双光子吸收截面. 因此，分子的对称性是否比不对称性更有利于增大分子的双光子吸收截面，还与分子的π中心部分的特性有关. 还给出了电荷转移态的电荷迁移过程. 关键词： 双光子吸收 响应函数方法 非线性光学     

Third-Order Nonlinear Optical Properties of a Series of Polythiophenes

The third-order nonlinear optical properties of a series of polythiophenes are investigated with the Z-scan method under picosecond pulse laser irradiation at 532nm. The copolymers exhibit a good nonlinear response： large nonlinear refraction coefficients without nonlinear absorption. The signs of nonlinear refraction coefficients are positive, which are opposite to the negative signs of the polythiophene reported before. The mechanism accounting for the process of nonlinear refraction under pulse laser excitation is analyzed from the viewpoint of the electrondonor/acceptor units of polythiophenes. Moreover, changes of nonlinearity according to the lengths of main chains in polythiophene molecules are discussed.     

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.     

Concentration dependent nonlinear refraction in chloroaluminum phthalocyanine/ethanol solution

Nonlinear refractive properties of chloroaluminum phthalocyanine (CAP) in ethanol solution are studied using the Z-scan technique with picosecond (ps) and nanosecond (ns) laser pulses at a wavelength of 532 nm. A transition from self-focusing to self-defocusing in CAP solution excited by 10 ns pulses is observed during the decrease of its concentration. This transition is due to co-existing excited-state refraction and transient thermal lensing effects. The experimental results are described very well using the rate-equation model and the theory of transient thermal refraction in liquids. The refractive cross sections of the excited-state are also obtained.