飞秒激光激发下本征GaP非线性吸收及Kerr效应的实验研究

采用掺镱光子晶体光纤飞秒激光放大器为抽运源,搭建了偏振分辨的Z-scan实验系统.实验研究了块状本征磷化镓(GaP)晶体的非线性吸收和非线性折射率系数.研究证明,在中心波长1 μm飞秒激光的作用下,本征GaP晶体的非线性吸收主要为三光子吸收.而且还表明本征GaP的非线性吸收和非线性折射率系数具有很强的各项异性、偏振相关性及饱和特性. 关键词： 磷化镓 Z-scan Kerr效应 三光子吸收     

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.     

NLO characteristics of D-π-A coumarin-thiophene bridged azo dyes by Z-scan and DFT methods

ABSTRACT

The structural, electronic, intramolecular charge transfer (ICT) and nonlinear optical (NLO) properties of the donor-π-acceptor (D-π-A) azo linked dyes bearing coumarin thiophene bridge with different acceptors were inspected by Z-scan and DFT methods. The dye 3a exhibits bathochromic absorption maxima (649 and 650?nm) in the near IR region in DMF and DMSO. The dye 3a holds low HOMO–LUMO gap elucidated by CV and DFT indicating strong ICT character. The thermal stability is high for 3a and it shows enhanced NLO property by Z-scan and DFT methods as predicted in both global and range-separated hybrid functionals. The molecular geometry was optimised using B3LYP/6-311?+?g(d,p). The ICT characteristics are correlated with NLO properties obtained by Z-scan and DFT techniques.     

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。     

聚-10,12-二十五碳双炔酸Langmuir-Schaefer膜的非线性光学性质

通过飞秒脉冲激光单光束Z 扫描方法研究了聚 10,12 二十五碳双炔酸Langmuir Schaefer膜在非共振吸收区的三阶非线性光学特性。钛蓝宝石激光器的输出脉宽为60～70fs、波长为800nm,在入射光平均功率为145mW时测得其三阶非线性极化率为5.33×10-9esu。这一结果较该类材料的有掺杂的薄膜明显增强,与微晶和单晶达到同样的量级,对此进行了分析和讨论。     

四磺化酞菁氧钒自组装膜的三阶非线性光学性能研究

为提高金属酞菁膜的三阶非线性光学性质,采用静电自组装技术制备出了包含阴离子四磺化酞菁氧钒(VOTsPc)和阳离子聚乙烯亚胺(PEI)交替层的复合薄膜.通过紫外-可见光谱仪表征了VOTsPc/PEI交替多层组装体的组装过程,结果表明组装过程为有规律的连续吸收过程.利用原子力显微镜技术研究了VOTsPc/PEI薄膜的表面形貌,结果表明膜表面是光滑的、均匀的;膜表面紧密堆积了纳米级颗粒,平均粒径为75 nm,平均表面粗糙度为4.406 nm.使用调Q倍频ns/ps Nd∶YAG脉冲激光系统,在输出激光波长为532 nm,脉冲宽度为4 ns条件下,通过Z-扫描测试研究了组装膜的三阶非线性光学性质.通过对实验数据的模拟和计算,30-双层VOTsPc/PEI膜的非线性极化率n2和非线性吸收系数β值分别为4.87×10-6esu和1.2×10-5m/W,三阶非线性极化率χ(3)值为1.57×10-6esu.VOTsPc/PEI膜显示出较强的非线性反饱和吸收性能,具有广阔的应用前景.     

六棱柱型金属团簇化合物Mo2Ag4S8(dppy)4的合成与非线性光学性质

新合成了一种六棱柱型金属团簇化合物Mo2Ag4S8(dppy)4, 并用X射线单晶衍射结构分析方法测定了其晶体结构. 应用Z-scan技术研究了该金属团簇化合物在波长为532 nm的纳秒激光脉冲作用下的三阶非线性光学特性. 为了研究Mo2Ag4S8(dppy)4的非线性起源, 应用泵浦探测技术研究了该金属团簇化合物在波长为532 nm的皮秒激光脉冲作用下的光学非线性响应. 实验结果表明金属团簇化合物Mo2Ag4S8(dppy)4具有自聚焦特性和非线性吸收特性; 非线性折射率n2, 非线性吸收系数β和非线性极化率χ(3)分别为1.45×10－10 esu, 6.2×10－10 m/W及2.1×10－11 esu. 实验结果表明金属团簇化合物Mo2Ag4S8(dppy)4的光学非线性响应是非线性吸收和非线性散射共同作用的结果.     

π-Conjugated Unit-Dependent Optical Properties of Linear Conjugated Oligomers

The optical properties of three linear conjugated oligomers （F-P, F-P-F, and P-F-P-F-P）, where phenothiazine （P） and fluorene （F） groups arrange alternately, are investigated. With the enhancement of the π-conjugated system, their absorption and emission bands both gradually red shift, and their two-photon properties are also improved. Meanwhile, their fluorescence dynamic traces are analyzed with continuous rate distribution model, exhibiting that their decay rates gradually accelerate and the rate distribution width become narrower. The quantum chemical calculation offers their molecular structures and transition mechanism, showing that the enhancement of π-conjugated system should be responsible for tile improvement of two-photon properties.     

以衍射理论为基础考虑双光子吸收的Z-扫描理论

以菲涅尔-基尔霍夫衍射理论为基础,建立了非线性介质对高斯光束的衍射模型,对高斯光束通过非线性介质后的传输行为进行了详细的理论推导和数值计算,从一种新的角度解释了Z-扫描现象.理论推导出了考虑双光子吸收的闭孔和开孔Z-扫描曲线的统一公式,是计算非线性折射率和双光子吸收系数的一种新方法.数值模拟计算表明,对于考虑双光子吸收的闭孔Z-扫描曲线,其结果与经典的Z-扫描理论完全一致.而对于已给定的开孔Z-扫描曲线,用该理论计算出的双光子吸收系数是经典开孔Z-扫描理论计算值的1/3,其它结论与传统Z-扫描理论完全吻合.该理论的近似条件只要求薄样品和小非线性吸收,比传统理论具有更好的准确性.     

二茂铁基查尔酮衍生物的超快三阶非线性光学响应

合成三例二茂铁基查尔酮衍生物:1-二茂铁基-3-(5-溴噻吩-2-基)-2-丙烯-1-酮(1)、1-二茂铁基-3-(4-溴噻吩-2-基)-2-丙烯-1-酮(2)和1-二茂铁基-3-(5-氯噻吩-2-基)-2-丙烯-1-酮(3);采用1H NMR、13C NMR和HR-MS对化合物1～3进行了结构表征,并测定了其热学性质;运用密度泛函理论方法进行结构优化,并计算得到了它们的分子轨道能量和极化率;采用紫外-可见吸收光谱与Z-扫描技术(532nm,180fs)分别测定了三种化合物的线性和非线性光学性质。结果表明,化合物1～3的紫外吸收波长发生明显红移,且1的非线性吸收幅度、极化率和分子超极化率最大; 1、2和3均存在分子内电荷转移现象,表现出超快三阶非线性光学响应。