Kinetics of generation, relaxation, and accumulation of electronic excitations under two-photon interband picosecond absorption in tungstate and molibdate crystals

Under two-photon 523.5 nm interband picosecond laser excitation, we measured the kinetics of induced absorption in PbWO₄, ZnWO₄, and PbMoO₄ crystals with 532 to 633 nm continuous probe radiation. We obtained real-time information about the dynamics of the generation, relaxation, and accumulations of electronic excitations over a wide time range (from picoseconds to hundreds of seconds) and the 77–300 K temperature range. For the studied crystals, exponential temperature-independent growth of the induced absorption (IA) with 60 ns rise time reflects the dynamics of the generation of electronic excitation. The kinetics of the IA exponential growth with temperature-dependent 3.5–11 μs time constants reflect the dynamics of energy migration between neighboring tungstate (molibdate) ions to traps for the studied crystals. The multiexponential relaxation absorption kinetics strongly depend on temperature, and the relaxation decay time of induced absorption increased from tens to hundreds of milliseconds to seconds under crystal cooling from 300 to 77 K. We found that the increase in the laser pump repetition rate (0–10 Hz) leads to the accumulation of electronic excitations. Control of the repetition rate and the number of excitations allowed us to change the relaxation time of the induced absorption by more than two orders of magnitude. Due to accumulation of excitations at 77 K, the absorption relaxation time can exceed 100 s for PbWO₄ and PbMoO₄ crystals. In the initially transparent crystals, two-photon interband absorption (2PA) leads to crystals opacity at the 523 and 633 nm wavelengths. (An inverse optical transmission of the crystals exceeds 50–55 at a 50–100 GW/cm² pump intensity.) Measured at ～1 mW probe radiation of 532 and 633 nm wavelengths, the induced absorption values are comparable with those obtained under two-photon absorption at ～5 kW pump power. An optical 2PA shutter for the visible spectral range is proposed with a variable shutting time from hundreds of microseconds to tens of seconds.     

Rapid formation kinetics of a long-lived electron-hole drop in Ge under pulsed excitation

The buildup of a large long-lived electron-hole drop in stressed Ge is studied using its Alfvén wave resonances. This microwave method permits rapid time resolution of the formation process after a short intense (100 nsec, 7 W) laser excitation pulse. A delay of about 1 μsec is observed before the drop radius rapidly increases from zero to ～ 100 μm within the next μsec. This is consistent with the interpretation that the photo-produced electron-hole pairs are quickly accelerated to the strain-induced potential minimum which is well within the crystal.     

Recombination luminescence lifetimes and the self-trapped excition in alkali halides

The decay of recombination luminescence in undoped KI and RbI at low temperatures has been measured following pulsed excitation by two-photon absorption and other methods. Several distinct exponential components are observed whose decay times vary with temperature. The most notable case is the principal component of the intrinsic luminescence in KI, whose decay time increases exponentially from 2 μsec at 12 K to 280 μsec at 1.38 K. The data are accounted for in terms of changing populations within a zero-field-split triplet state of the self-trapped excition. Evidence concerning the origin of a second luminescent triplet state in KI, RbI, and CsI is discussed; this state is similar to those of the self-trapped excition, but may involve an extrinsic perturbation.     

Ultrafast carrier dynamics of Cu2O thin film induced by two-photon excitation

Cuprous oxide (Cu₂O) has attracted plenty of attention for potential nonlinear photonic applications due to its superior third-order nonlinear optical property such as two-photon absorption. In this paper, we investigated the two-photon excitation induced carrier dynamics of a Cu₂O thin film prepared by radio-frequency magnetron sputtering, using the femtosecond transient absorption experiments. Biexponential dynamics including an ultrafast carrier scattering (< 1 ps) followed by a carrier recombination (> 50 ps) were observed. The time constant of carrier scattering under two-photon excitation is larger than that under one-photon excitation, due to the different transition selection rules and smaller absorption coefficient of the two-photon excitation.     

基于光谱吸收法和荧光法的甲烷和二氧化硫检测系统的研究

根据污染气体的光谱吸收特性与荧光特性,设计了一套时分复用检测系统,既可以使用光谱吸收法检测甲烷和二氧化硫又可以使用荧光法检测二氧化硫。系统采用组合可切换光源、共用光路、气室及信号处理部分,首先进行光谱吸收和荧光的特性测量,然后进行光谱吸收法检测甲烷与二氧化硫浓度实验,以及紫外荧光法检测二氧化硫浓度实验。经过光谱吸收和荧光的特性测量得出吸收法测二氧化硫和甲烷的吸收峰处的激发波长分别为280nm和1.64μm,荧光法测二氧化硫最佳激发波长为220nm。经光谱吸收法实验可得甲烷浓度与相对强度的线性关系和二氧化硫浓度与输出电压的线性关系,线性度分别为98.7%,99.2%;经荧光法实验可得二氧化硫浓度与电压成线性关系,线性度达到了99.5%。研究表明,该系统能使用于污染气体的光谱吸收检测和紫外荧光检测。将两种测量方式组合在一起,降低了成本与体积,同时此系统也可用于其他气体的检测,有一定的应用价值。     

Pump power dependence of the electron-hole plasma luminescence in Ga-doped ZnO film

Time resolved two-photon absorption induced electron-hole plasma (EHP) luminescence of Ga-doped ZnO thin film was measured by an ultrafast optical Kerr gate (OKG) in femtosecond time regime. Experimental results showed that the buildup time of the EHP luminescence was strongly dependent on the excitation fluence. The dependence of the buildup time of EHP on excitation fluence probably arose mainly from the relaxation of the hot carriers due to the carrier-carrier interaction, which increased with the increase of excitation fluence.     

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。     

双光子激发ZnSe自由载流子超快动力学研究

采用Z扫描和抽运-探测实验技术, 在波长为532 nm、脉冲宽度为41 fs的条件下测得ZnSe晶体的双光子吸收系数, 并获得了不同激发光强下的自由载流子吸收截面、电子-空穴带间复合时间和电子-声子耦合时间. 研究发现, 随着激发光强的增大, 自由载流子吸收截面减小, 复合时间变短. 当激发光强增大导致载流子浓度大于10¹⁸ cm^-3时, 抽运-探测信号出现明显改变, 原因归结为强光场激发导致样品在短时间内带隙变窄和电子-空穴等离子体的形成.     

Nonlinear Bragg structures based on ZnS/ZnSe superlattices

Nonlinear optical response of periodic ZnSe/ZnS heterostructures is reported using interband excitation of a ZnSe sublattice by nano-, pico- and femtosecond laser pulses. A considerable shift of the reflection spectrum and large relative reflection changes were observed in a wide spectral range corresponding to the transparency region of ZnSe far from the intrinsic absorption onset. Evaluated refraction-index change is about −0.05 with the relaxation time being about 3 ps. In the case of femtosecond excitation, a wide-band nonlinear response is observed for both one-photon near-UV and two-photon near-IR excitation. The nonlinear refraction is supposed to be controlled by population-induced absorption changes in ZnSe single crystals and relevant refraction-index modification via Kramers–Kronig relations. The nonlinearity relaxation time is supposed to trace a transition from a non-equilibrium to a quasi-equilibrium distribution of electrons and holes within ZnSe conduction and valence bands, respectively, rather than the electron–hole recombination time. The nonlinearity mechanism does not reduce to just population-dependent absorption saturation, but essentially results from the specific distribution function in the first instance after excitation.     

Spectroscopic measurements on a titanium plasma gun with hydrogenated electrodes

The plasma produced by a plasma gun which consists of concentric titanium and tantalum washers has been observed in the plasma gun as well as in a drift tube in which the plasma particles have been injected. Axial drift velocities of hydrogen and impurities have been determined in the drift tube by optical time-of-flight measurements. Maximum hydrogen velocities between 9·10⁶ to 1·10⁸ cm/sec could be determined, in agreement with magnetic probe-, Faraday cup-, microwave-, and electrostatic energy analyser measurements. The plasma which is produced within the plasma gun by a powerful discharge (vacuum arc) has been observed with a framing camera, spectrographs and photomultipliers. From end-on observed time resolved spectrograms the temperatures and electron densities have been determined as a function of time. The measurements indicate that thermal equilibrium is reached about 2·5 μsec after the firing of the main discharge. 4 μsec after the beginning of the main discharge a maximum temperature of about 72000° K is reached. The measurements further indicate that the high-energy part of the ejected particles is produced before an equilibrium state in the plasma gun has been established.     

BaF2替代BaO 对钡镓锗酸盐玻璃光学性质的影响

在摩尔分数组成x(BaO),r(Ga2O),r(GeO2)为0．20,0．15,0．65的玻璃中,分别以摩尔分数0．05,0．10．0．15和0．20的BaF2替代BaO,研究了氟化物对玻璃折射率和光吸收性质的影响。结果表明,在玻璃中加入氟化物．玻璃折射率和色散降低,玻璃的紫外吸收边向短波侧迁移,而红外吸收边无明显变化。不含氟化物的氧化物玻璃中含有大量的OH基．这些OH基在2．24μm、2．97μm和4．23μm附近引起光吸收．在含氟化物的玻璃中,2．24μm的吸收峰消失,而2．97μm和4．23μm附近的吸收大大减弱。讨论了各OH基吸收峰的起源,利用计算机技术对2．97μm附近的OH基吸收峰进行了高斯峰分离。玻璃在2．24μm的弱吸收可能来自H2O分子的一个伸缩模和两个振动模的结合(p 2ρ)．4．23μm吸收带是由与非桥O形成强氢键的OH基(T-OH…O^--T)伸缩振动引起,而中心位于2．7～3．2μm的OH吸收带为受不同程度氢键影响的OH基伸缩振动吸收．这些吸收带叠加导致OH吸收带出现非对称性加宽,吸收中心随玻璃中OH含量不同发生移动。     

聚丁二炔Langmuir—BLodgett薄膜的光声谱研究（Ⅱ）光谱综合分析和荧 …

本文用光声谱结合光吸收谱,荧光光谱等对在工业上在潜在应用前景的聚十炔（ｐｏｌｙｄｉａｃｅｔｙｌｅｎｅ,ＰＤＡ）Ｌａｎｇｍｕｉｒ－Ｂｌｏｄｇｅｔｔ（ＬＢ）薄膜进行了研究。     

聚丁二炔Langmuir-Blodgett薄膜的光声谱研究(Ⅱ) 光谱综合分析和荧光量子效率

本文用光声谱（ｐｈｏｔｏａｃｏｕｓｔｉｃｓｐｅｃｔｒｏｓｃｏｐｙ,ＰＡＳ）结合光吸收谱、荧光光谱等对在工业上有潜在应用前景的聚丁二炔（ｐｏｌｙｄｉａｃｅｔｙｌｅｎｅ,ＰＤＡ）Ｌａｎｇｍｕｉｒ－Ｂｌｏｄｇｅｔ（ＬＢ）薄膜进行了研究。对经不同气体环境处理的ＰＤＡＬＢ膜的紫外－可见光声谱、光吸收谱和荧光光谱的综合分析表明,ＰＤＡＬＢ膜的激发态弛豫过程中激子和极化子形成的元激发性质。此外,还讨论了ＰＤＡＬＢ膜的荧光量子效率。本文的研究结果表明,用光声谱研究ＬＢ膜,可以获取仅用其他光谱得不到的信息。     

Laser-induced spectral broadening and hole-burning in rare earth doped crystals and coherent optical spectroscopy for frequency upconversion

The excitation spectra for linear fluorescence and for frequency upconversion are recorded in Er³⁺ doped crystal Er:YAG. An excitation induced spectral broadening and hole-burning are shown to appear at the resonant frequency of the linear fluorescence excitation spectrum, where the upconversion is simultaneously enhanced. Rate equation analysis is applied to model the optical pumping processes in the crystal. We present evidence that the induced resonance broadening and hole-burning are the result of excitation competition between the linear absorption and the excited state absorption. Femtosecond pulse pairs are applied to excite the linear and nonlinear frequency conversion, resulting in coherent controlled branching ratio between the linear and nonlinear frequency conversion. The experimental reasults are in good agreement with the numerical evaluation based on optical Bloch equation. PACS 78.47.+p; 42.65.Re; 78.20.Ci     

高功率脉冲电子束辐照SiO$lt;sub$gt;2$lt;/sub$gt;的光学和激光损伤性能

研究了不同剂量的60 kW高功率脉冲电子束辐照对高纯熔石英玻璃的微观结构、光学性能和激光损伤特性的影响规律. 光学显微图像表明, 辐照后熔石英样品由于热效应导致表面破裂, 裂纹密度和尺寸随辐照剂量增加而增大, 采用原子力显微镜分析表面裂纹的微观形貌, 裂纹宽度约1 um, 同时样品表面分布着大量尺寸约0.1–1μm的碎片颗粒. 吸收光谱测试表明, 所有样品均在394 nm处出现微弱的吸收峰, 吸收强度随着电子束辐照剂量增大呈现先增加后减小的趋势. 荧光光谱测试发现辐照前后样品均有3个荧光带, 分别位于460, 494和520 nm, 荧光强度随辐照剂量的变化趋势与吸收光谱一致. 利用355 nm激光研究了不同剂量电子束辐照对熔石英激光损伤阈值的影响, 结果表明熔石英的损伤阈值随着辐照剂量的增加而降低. 在剂量较低时, 导致熔石英激光损伤阈值下降的原因主要是色心缺陷; 剂量较高时, 导致损伤阈值降低的原因主要是样品表面产生的大量微裂纹和碎片颗粒对激光的调制和吸收. 关键词： 熔石英 电子束辐照 色心 激光损伤阈值     

Laser excitation spectra and lifetimes of CBrCl and CBr2 in solid Ar

The CBr₂ and CBrCl emissions in solid Ar have lifetimes of 5.6 and 14.5 μsec, respectively. Laser excitation spectra of the fluorescence provide information about the upper state vibrations structure of these species. Mode-to-mode vibrational energy transfer in CBrCl appears to be inefficient.     

Sub-wavelength probing and modification of photonic crystal nano-cavities

In this work we present a sizeable and reversible spectral tuning of the resonances of a two-dimensional photonic crystal nano-cavity by exploiting the introduction of a sub-wavelength size glass tip. The comparison between experimental near-field data and results of numerical calculations shows that the spectral shift induced by the tip is proportional to the local electric field intensity of the cavity mode. This observation proves that the electromagnetic local density of states in a microcavity can be directly measured by mapping the tip-induced spectral shift with a scanning near-field optical microscope. Moreover, a non-linear control on the cavity resonance is obtained by exploiting the local heating induced by near-field laser excitation at different excitation powers. The temperature gradient due to the optical absorption results in an index of refraction gradient which modifies the dielectric surroundings of the cavity and shifts the optical modes.     

Reverse-saturable absorption in aluminophthalocyanine-doped xerogels

Aluminophthalocyanines were encaged in different silica xerogel matrices. Nonlinear reverse-saturable absorption behavior was observed for both nanosecond and picosecond pulse excitation at 532 nm. In order to determine the relaxation paths of the molecules after optical excitation, we measured the evolution of the transmission of a continuous probe beam through the samples following absorption induced by a pump pulse. The transmission recovery was a few tens of microseconds. The fluorescence lifetime was about 10 ns.     

单光子和双光子激发的超歧化聚合物的光谱学特性研究

研究了二种新型超歧化聚合物在氯仿和二甲基甲酰胺溶剂中的飞秒激光单光子和双光子激发的光谱学特性．这二种聚合物是以苯为核、以对二甲氧基苯为连接单元，分别以二甲基苯胺为端基或以特丁基苯为端基的超歧化共轭聚合物．结果表明这种超歧化聚合物具有较大的溶剂极性相关的飞秒双光子吸收截面，不同的端基不仅影响分子内的电荷转移，而且导致超歧化分子共轭程度的变化．作为一种潜在的光学非线性材料，利用这种大的双光子吸收截面的超歧化聚合物可实现了飞秒双光子直写的三维高密度数据存储．     

Nonresonant and Resonant Nonlinear Absorption of CdSe-Based Nanoplatelets

We present a comprehensive understanding of the nonlinear absorption characteristics of CdSe-based nanoplatelets(NPLs) synthesized by the solution-phase method and the colloidal atomic layer deposition approach through Z-scan techniques at 532 nm with picosecond pulses. The CdSe NPLs exhibit strong two-photon induced free carrier absorption(effective three-photon absorption) upon the nonresonant excitation, resulting in a remarkable optical limiting behavior with the limiting threshold of approximately 75 GW/cm~2. A nonlinear optical switching from saturable absorption(SA) to reverse saturable absorption(RSA) with increasing the laser intensity is observed when coating CdSe NPLs with a monolayer of CdS shell to realize the resonant absorption. The SA behavior originates from the ground state bleaching and the RSA behavior is attributed to the free carrier absorption.These findings explicitly demonstrate the potential applications of CdSe-based NPLs in nonlinear optoelectronics such as optical limiting devices, optical pulse compressors and optical switching devices.