Investigation of optical nonlinearities in Pd(po)2 by Z-scan technique

With nanosecond scale at a 532 nm wavelength, we firstly measured the nonlinear optical absorption and refraction coefficients of Pd(po)₂ complex by using Z-scan technique, here Hpo=1-hydioxy-2-pyridone. We describe an empirical expression for the case when nonlinear refraction is accompanied by nonlinear absorption to separately evaluate the nonlinear refraction and the nonlinear absorption by performing straightforward measurements with the aperture removed. The nonlinear optical response of Pd(po)₂ was determined by the linear decreasing irradiance-dependence. The nonlinear absorption originates from the near resonant two-photon absorption while the mechanism of the nonlinear refraction is the near resonant two-photon absorption transition enhancement. The linear increasing dependences of the optical nonlinearities on the incident irradiance arise from the population redistribution due to the near resonant two-photon absorption.     

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.     

Effect of nonlinear absorption in estimation of order of nonlinear optical process by fluorescence intensity

We report the effect of nonlinear absorption on the fluorescence signal. Attenuation of the incident beam intensity (I) in the medium due to nonlinear absorption reduces the fluorescence signal. We show that fluorescence signal proportional to I² is not always indicative of two-photon absorption process but such a dependence can be obtained for three or four-photon absorption process due to attenuation of the pump beam by nonlinear absorption. This reduction in the fluorescence signal due to nonlinear absorption is found to be more sensitive in the higher order nonlinear optical processes.     

The study of the nonlinear absorption in the nonlinear-imaging technique with phase object

The nonlinear absorption can produce a nonlinear image very similar with the one created by the nonlinear refraction when using the nonlinear-imaging technique with phase object to measure the third-order nonlinearity of materials, but the principles of them are different. The formation of the nonlinear absorption image is explained, and the condition that the highest sensitivity of the nonlinear absorption measurement can be reached is deduced. For the materials with both nonlinear absorption and refraction, we find a proper phase shift of the phase object where the effect of the nonlinear refraction to the measured signal can be eliminated. The nonlinear absorption and refraction are numerically simulated when the phase shift of phase object to be π/2 that is normally used. The qualitative tendency of the signal variation is presented.     

Effect of self assembly on the nonlinear optical characteristics of ZnO thin films

In the present work, we report the third order nonlinear optical properties of ZnO thin films deposited using self assembly, sol gel process as well as pulsed laser ablation by z scan technique. ZnO thin films clearly exhibit a negative nonlinear index of refraction at 532 nm and the observed nonlinear refraction is attributed to two photon absorption followed by free carrier absorption. Although the absolute nonlinear values for these films are comparable, there is a change in the sign of the absorptive nonlinearity of the films. The films developed by dip coating and pulsed laser ablation exhibit reverse saturable absorption whereas the self assembled film exhibits saturable absorption. These different nonlinear characteristics in the self assembled films can be mainly attributed to the saturation of linear absorption of the ZnO defect states.     

非线性吸收对多组分气体分析的影响及其修正方法

利用非分散红外(NDIR)技术研究了非线性吸收现象对多组分气体分析交叉干扰扣除的影响及其修正方法。理论上推导了由于非线性吸收导致的干扰系数变化对系统测量准确度的影响。对常规的干扰方程组进行了修正,使用干扰函数来定量分析气体间的交叉干扰,当测量气体存在非线性吸收时,干扰函数也会发生相应变化。基于最小二乘法,以三阶多项式为拟合模型,拟合出了系统的干扰函数。利用拟合的干扰函数,通过实验证明了提出的修正方法在系统存在非线性吸收现象时仍能有效地扣除气体间的交叉干扰。     

Effect of picosecond radiation intensity on nonlinear absorption of glasses with silver nanoparticles

The dependence of the process of nonlinear absorption on the intensity of laser radiation of a picosecond duration was studied with the use of the second harmonic of a Nd:YAG laser (λ = 532 nm, τ = 55 ps). The values of the nonlinear absorption coefficient and of the imaginary part of the third-order nonlinear susceptibility of materials were measured. The nonlinearity of absorption in the materials under study was found to be caused by the saturation of absorption.     

1-(2-吡啶偶氮)-2-萘酚薄膜的非线性光学特性研究

运用Ｚ扫描方法研究了１－（２－吡啶偶氮）－２－萘酚薄膜的非线性光学特性。用皮秒脉冲激光测得在５３２ ｎｍ 处、光强较低时χ（３）Ｒ ＝ １．２９×１０－ ９ ｅｓｕ, β＝ ４２ ｃｍ ／ＧＷ; 同时研究了不同光脉冲能量时的非线性吸收特性, 发现其非线性吸收随着光强的增大由反饱和吸收转为饱和吸收     

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.     

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.     

Third-Order Nonlinear Optical Susceptibility of Indium Phosphide Nanocrystals

InP nanocrystals synthesized by refluxing and annealing of organic solvent are determined from XRD measurements to have an averse granularity of 25 nm. The nonlinear optical properties of the InP nanocrystals studied by using laser Z-scan technique with 50 ps pulses at 532nm are found to reveal strong nonlinear optical properties and two-photon absorption phenomenon. Also, the nonlinear absorption coeffcient, the nonlinear refractive index and the third-order nonlinear optical susceptibility are determined by experiments, in which the nonlinear refractive index is three orders of magnitude larger than that of bulk InP.     

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。     

铝镓氮薄膜双光子吸收效应

基于飞秒激发Z扫描实验技术,研究了氮化镓薄膜和不同铝掺杂含量的掺铝氮化镓(以下简称铝镓氮)薄膜的超快非线性光学响应特性。在开孔Z-scan测试中,纯Ga N晶体薄膜表现出典型的双光子吸收特性,双光子吸收系数为3.5 cm/GW,且随着激发光强的增大而逐渐减小。随后测试了不同铝掺杂含量的Al_xGa_(1-x)N薄膜的非线性吸收系数。结果表明,随着铝掺杂摩尔分数的提高(0,19%,32%,42%),非线性吸收系数逐渐减小(18,10,6,5.6 cm/GW)。结合半导体非线性吸收理论分析,Al_xGa_(1-x)N薄膜材料的非线性过程主要是双光子吸收主导非线性响应物理过程。实验结果与半导体双光子吸收过程Sheik-Bahae理论符合得很好。     

Investigation of nonlinear optical properties of various organic materials by the Z-scan method

We have studied the nonlinear optical properties of various organic materials (vegetable oil, juice, wine, cognac, Coca-Cola and Fanta drinks, Nescafé coffee, tea, gasoline, clock oil, glycerol, and polyphenyl ether) that are used in everyday life. Their nonlinearities have been studied by the Z-scan method in the near-IR and visible spectral ranges. We have shown that the majority of samples possess a nonlinear absorption; however, some of the studied materials show a strong saturated absorption and nonlinear refraction. Red wine and glycerol proved to be the most interesting materials. For these samples, we have observed a change in the sign of the nonlinear absorption with increasing laser intensity, which was attributed to the competition between two-photon absorption and saturated absorption.     

Nonlinear optical behaviours in a silver nanoparticle array at different wavelengths

The optical nonlinearities of an Ag nanoparticle array are investigated by performing the Z-scan measurements at the selected wavelengths (400, 600, 650, and 800 nm). The nonlinear refraction index in the resonant region (around 400 nm) exhibits a significant enhancement by two orders compared with that in the off-resonant region (around 800 nm)), and exhibits an sign alternation of the resonant nonlinear absorption, which results in a negligible nonlinear absorption at a certain excitation intensity. Moreover, a low degree of nonlinear absorption was measured at the edges of the resonant region (600 and 650 nm), which is attributed to the competition of the saturated absorption and the two-photon absorption processes.     

Nonlinear optical behaviors in a silver nanoparticle array at different wavelengths

The optical nonlinearities of an Ag nanoparticle array are investigated by performing Z-scan measurements at the selected wavelengths (400, 600, 650, and 800 nm). The nonlinear refraction index in the resonant region (around 400 nm) exhibits a significant enhancement by two orders compared with that in the off-resonant region (around 800 nm)), and exhibits an sign alternation of the resonant nonlinear absorption, which results in a negligible nonlinear absorption at a certain excitation intensity. Moreover, a low degree of nonlinear absorption was measured at the edges of the resonant region (600 and 650 nm), which is attributed to the competition of the saturated absorption and the two-photon absorption processes.     

强非线性吸收下高斯光束Z-扫描衍射理论模型

 摘要：在同时考虑非线性折射和非线性吸收的情况下，借助光的衍射理论，研究了Z-扫描技术的衍射理论模型，分析了非线性折射和非线性吸收同时存在时Z-扫描曲线的形状特征和变化规律。数值计算表明，非线性吸收相移和非线性折射相移的比值是影响接收小孔输出光功率的重要因素。要想得到好的光限幅效果，应选取非线性相移比值远小于1或远大于2的非线性材料。     

Ultrafast nonlinear optical response of carbon nanotubes functionalized with water soluble porphyrin

A new nanocomposite is obtained by functionalizing carbon nanotubes (CNTs) with a water soluble metalloprophyrin using a simple chemical technique and characterized by optical absorption, IR, and Raman spectroscopy. Results from spectroscopic studies indicate the noncovalent nature of interaction between CNTs and porphyrin. The ultrafast nonlinear response is characterized by measuring the nonlinear absorption coefficient and refractive index by z-scan technique in the femtosecond pulse regime. The nanocomposite is found to exhibit two-photon absorption (TPA) with a reasonably large nonlinear optical coefficient, whereas pure CNTs is known to exhibit saturable absorption. Design of such water soluble nanocomposites offers scope for obtaining materials with enhanced ultrafast optical nonlinearity.     

Absorption of finite amplitude focused ultrasound

Predictions of the absorption of focused finite amplitude waves based on weak shock theory have been tested experimentally. The characteristics of this absorption are qualitatively different from those associated with small signal losses. Under appropriate conditions, the absorption of finite amplitude ultrasound is determined largely by source amplitude, field geometry, and the nonlinear properties of the medium and is only weakly dependent upon the small signal absorption coefficient of the material. These effects are seen most dramatically in sharply focused sound fields. To emphasize nonlinear absorption in an experimental test of these predictions, measurements of heating were made in agar which has a very small linear absorption coefficient. Under appropriate conditions, nonlinear losses can make the effective absorption coefficient of this poorly absorbing material somewhat greater than the soft tissues of the body.     

溶剂对光致变色材料-乙基红的光学特性影响

研究了溶剂性质对光致变色材料乙基红光学性质的影响.用吸收谱测定了乙基红染料在不同溶剂中的溶剂化位移.对相同浓度多种乙基红溶液进行了Z-scan测量,测量了不同乙基红溶液的光限幅效应,并讨论了其与溶剂之间的关系.随极性增加,吸收谱蓝移,可以通过选择不同溶剂,改变非线性材料的应用窗口.实验结果表明,在连续光照射下,乙基红溶液的非线性折射主要由热效应引起,非线性折射系数n2受溶剂的热学性质影响较大.此外,Z-scan结果中的非线性吸收为饱和吸收.至于光限幅效应,主要受热效应影响,但亦可由吸收谱预测出在某波长处的动态范围.得出的结论有助于偶氮染料作为非线性材料的应用.