Broadband saturable absorber with cobalt-doped tellurite glasses

A robust solid-state saturable absorber was developed with cobalt-ion-doped tellurite glasses that has a broad saturable-absorption band in the near-infrared. A nonlinear optical absorber was measured by the Z-scan technique. Numerically fitting the Z-scan experimental data yields excited-state absorption cross sections at a 1064-nm laser wavelength of sigma(es) = 1.45 x 10(-20) and sigma(es) = 1.15 x 10(-20) cm2 for 1.0- and 2.5-at. % Co2+-doped glasses, respectively.     

Reverse saturable absorption in chlorophyll A solutions

The dynamic nonlinear absorption of a chloroform solution of chlorophyll A was investigated using the Z-scan technique with picosecond pulses at 532 nm. The nonlinear absorption exhibits a reverse saturation, indicating a strong intersystem crossing (singlet–triplet) process. The time evolution of the optical nonlinearity, modeled by means of a five-level energy diagram, allows the determination of excited-state cross sections and the lifetime of the intersystem crossing based on its absorption characteristics and efficient formation of triplet states. Chlorophyll A was found to be a good candidate for a sensitizer in photodynamic therapy. Received: 14 February 2002 / Published online: 2 May 2002     

芘四磺酸四钠盐光物理性质的研究

本文利用吸收光谱、荧光光谱以及时间分辨瞬态吸收光谱研究芘四磺酸四钠盐的光物理特性.研究结果表明,芘四磺酸四钠盐在水溶液中的荧光量子产额高达0.54.在纳秒时间分辨瞬态吸收光谱研究中发现芘四磺酸四钠盐具有很长的三重态寿命(3.5ms),这有利于将其作为光敏化分子把激发能传给其它受体分子;芘四磺酸四钠盐被光激发后,可能发生双光子吸收过程并产生芘四磺酸四钠盐阳离子,其吸收峰为460nm和505nm.由实验结果,我们给出了其动力学过程的解释.     

Experimental test of a four-level kinetic model for excited-state intramolecular proton transfer dye lasers

The nanosecond pulses of a dye laser oscillator based on the excited-state intramolecular proton-transfer reaction (IPT) of salicylamide and 2-hydroxylphenyl benzimidazole dyes have been studied as a function of several experimental parameters. To explain the operation of this laser a numerical four-level kinetic model was developed until the lasing properties of these dyes, in the presence of a variable oxygen concentration and pumped with a double pulse technique, could be reproduced. This was possible only by assuming that the efficiency of the laser is controlled by the absorption cross-section of a transient state with a lifetime in the nanosecond-picosecond range, which was tentatively identified as a ground state tautomeric species.     

Spectroscopy and continuous-wave diode-pumped laser action of Yb3+:YVO4

The growth, spectroscopic properties, and laser performance of Yb:YVO4 crystal with laser diode pumping are reported. A peak absorption cross section of 7.4 x 10(-20) cm2 at 985 nm, a radiative lifetime of 0.25 ms, and a stimulated-emission cross section of 1.25 x 10(-20) cm2 at 1008 nm for pi polarization were determined for the Yb3+ ions in YVO4. Continuous-wave laser action of Yb:YVO4 at 1020-1027 nm was demonstrated with an output power of 610 mW and a slope efficiency of 49%.     

Experiments with a high-density positronium gas

We have created a high-density gas of interacting positronium (Ps) atoms by irradiating a thin film of nanoporous silica with intense positron bursts and measured the Ps lifetime using a new single-shot technique. When the positrons were compressed to 3.3 x 10(10) cm-2, the apparent intensity of the orthopositronium lifetime component was found to decrease by 33%. We believe this is due to a combination of spin exchange quenching and PS2 molecule formation associated with colliding pairs of oppositely polarized triplet positronium atoms. Our data imply an effective cross section for this process of 2.9 x 10(-14) cm-2.     

β-胡萝卜素在乙腈体系中的激光光解研究

利用纳秒级激光光解瞬态吸收光谱装置,研究了以乙腈作为溶剂,以2-萘乙酮作为敏化剂的体系在355nm激光作用下敏化产生β-胡萝卜素激发三重态的机制,并进一步研究了β-胡萝卜素激发三重态的性质。研究显示2-萘乙酮和β-胡萝卜素的二元体系在355nm激光作用下,2-萘乙酮首先被激发为其激发三重态(420nm),2-萘乙酮激发三重态与β-胡萝卜素发生激发能转移,产生β-胡萝卜素激发三重态(510nm)。通过激发能转移的方法测得了β-胡萝卜素激发三重态在最大吸收波长510nm处的摩尔消光系数为23000L·mol-1·cm-1。改变β-胡萝卜素的浓度测得了其激发三重态在乙腈体系中的衰变反应速率常数6·5×104s-1,其在乙腈体系中的三重态寿命为15·6μs。同时获得了激发态2-萘乙酮与β-胡萝卜素之间激发能转移反应的速率常数1·5×1010L·mol-1·s-1。     

Cr^4＋：YAG可饱和吸收特性测量

测量了Cr4+:YAG材料的可饱和吸收特性,用多种数据分析方法处理了实验结果,Cr4+:YAG的基态吸收截面σgs=11×10-19cm2,激发态吸收截面σes=1.2×10-19cm2。     

金属卟啉化合物激发态折射与激发态吸收增强瞬态热折射竞争研究

应用激发态吸收增强瞬态热折射理论结合激发态折射理论研究了新型锌卟啉化合物Zn-porphyrin 中激发态吸收增强瞬态热折射与激发态折射间的相互竞争. 样品在不同脉宽激光激发下呈现自聚焦-自散焦间的转化. 当入射激光脉宽为4 ns时,激发态折射占主要地位,样品呈现自聚焦性质;当入射激光脉宽为8ns时,激发态吸收增强瞬态热折射占主要地位,激发态折射占次要地位,样品呈现自散焦性质. 关键词： 金属卟啉化合物 激发态折射 瞬态热折射     

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.     

Optical limiting and pulse reshaping of picosecond pulse trains by fullerene C60

We present a dynamical theory of nonlinear absorption and propagation of a laser pulse train that contains 20 subpulses with an individual pulse width of 100 ps. It is shown that the accumulative nonlinearity and the reverse saturation absorption play important roles in the optical limiting performance and pulse shaping. When the incident field is not too strong, the population transfer reveals a slow response process, and the periodic sequence of short light pulses can be regarded as a continuous long pulse. The general theory is applied to fullerence C₆₀, which is a popular reverse saturable absorption material and a good limiter because of its larger excited-state absorption cross-section compared with that of the ground state. The propagation of the front subpulses is mainly affected by the linear transition between the ground state and the first excited singlet state, while the latter subpulses are attenuated by the excited-state absorption. Moreover, these two different kinds of absorption mechanisms result in different radial distributions for different subpulses. The pulse propagation is studied by solving numerically the coupled rate equations and the propagation equation of the optical pulse intensity, using experimental parameters as input. We suggest a new method to measure the lifetime of the triplet state.     

Transient analysis of degenerate four-wave mixing in saturable absorbers: application to Cr:GSGG at 1.06 μm

We introduce a model of degenerate four-wave mixing in saturable absorbers in the transient regime when the interacting pulses have a duration much shorter than the lifetime of the excited-state level. Our model takes into account of the depletion and the mutual interaction of the pump waves. We study the influence of excited-state absorption on phase conjugate reflectivity. This theory agrees with experimental investigations made in Cr⁴⁺:GSGG with nanosecond pulses at λ₀ = 1.06 μm. A reflectivity of 0.6% is achieved and imaging capabilities are demonstrated.     

Time-resolved studies on the photoisomerization of a phenylene-silylene-vinylene type compound in its first singlet excited state

In femtosecond laser-flash photolysis experiments, the first singlet excited state of trans-ST, ((E,E)-{1,4-bis(2-dimethylphenylsilyl)ethenyl}benzene) showed a strong S1(π,π^?)-Sn absorption band at 540 nm in acetonitrile and at 550 nm in hexane. The lifetime of this state was determined to be 13.2±2.0 and 11.1±1.5 ps, respectively. Intersystem crossing was shown not to be a principal route for the deactivation of this S1 state of trans-ST. Evidence for this conclusion involved two complementary nanosecond laser-flash photolysis experiments. In one experiment involving direct excitation, no transient absorption spectrum was detected in the 350-650 nm spectral range. Yet, in the second experiment, on triplet sensitization, using xanthone, a transient absorption at 400 nm was tentatively assigned to the triplet state absorption of trans-ST. Photoisomerization was monitored in nanosecond time-resolved bleaching experiments. From these experiments the trans-cis photoisomerization quantum yield was determined to be 0.23 on direct trans-ST excitation. In a xanthone-sensitized stationary-state excitation experiment, the trans-cis isomerization quantum yield was determined to be 0.32. The main deactivation route of trans-ST in its S1 state is repopulation of the ground state directly through internal conversion or with the intermediacy of conformers with twisted geometry.     

有机材料反饱和吸收特性分析

从能级角度出发,结合入射激光脉宽对粒子吸收方面的影响,用速率方程模拟了各能级粒子数的瞬时变化关系,给出了激光脉宽与能级寿命可比拟时反饱和吸收的动态解,表明粒子在能级上的分布情况。用C60和HITCI(1,1′,3,3,3′,3′hexa methyl lindo tricarbocyanine Iodide)的实验参数理论模拟了激发态吸收截面大于基态吸收截面时透射率随光强的变化关系,用以说明大的上能级吸收截面可以抑制光强过大时引起的饱和吸收,增强材料的非线性光限幅特性。     

Cs(6P)激发态的辐射及与N2碰撞的能量转移

应用激光吸收和荧光方法,测量了Cs(6P)态与N2碰撞的精细结构转移和碰撞猝灭截面。Cs原子被激光激发到6P3/2态,将与泵浦激光束反向平行的检测激光束调到6PJ→8S1/2的跃迁,测量了6PJ激发态的密度及空间分布,由此计算了6PJ→6S的有效辐射率。在T=337 K(蒸气压公式给出Cs密度N0=1.25×1012cm-3)和N2密度2×1016相似文献   

Guiding of intense laser pulses in plasma waveguides produced from efficient, femtosecond end-pumped heating of clustered gases

We demonstrate intense pulse guiding in efficient femtosecond end-pumped waveguides generated in clustered gases. This novel scheme provides a route to significantly lower on-axis plasma density (< 10(18) cm(-3)) more than is feasible in conventional hydrodynamic plasma waveguides. Self-focused propagation and strong absorption of intense femtosecond laser pulses are used to produce long centimeter scale channels in an argon cluster jet, and a subsequent pulse is guided with 3 x 10(17) W cm(-2) intensity and approximately 50% coupling efficiency. Preliminary results with hydrogen clusters also show guiding.     

Energy transfer coupling of two-photon absorption and reverse saturable absorption for enhanced optical power limiting

We introduce a new approach to enhancing the optical power-limiting function at near-IR wavelength (~800 nm) by coupling effective two-photon absorption in one molecule with excited-state absorption in another molecule. We experimentally demonstrate this approach by using a strong two-photon absorbing dye, AF-380, and a strong reverse saturable absorber, C(60) . A nanosecond time-resolved experiment is used to show that energy transfer from AF-380 to C(60) generates triplet excitation in C(60) that further absorbs the pump beam to enhance the power-limiting function.     

Collision-induced vibrational energy transfer: K2[1(1) sigmau+ (nu'=2)]+He, H2-->K2[1(1) sigmau+(nu'=1,3)]+He, H2

Collisional energy transfer processes K2[1(1) sigmau+ (nu'=2)]+He, H2-->K2[1(1) sigmau+(nu'=1,3)]+He, H2 were studied by laser induced fluorescence under gas cell conditions. During the experiments, the cell temperature was kept constant at 420K. The buffer gas pressure was varied over the range from 40 to 250 Pa, Kz molecules were irradiated with pulses of radiation from an OPO laser, populating K2[1(1) sigmau+ (nu'=2)] by photon absorption. The resulting fluorescence included the direct component emitted in the decay of the optically excited state and the sensitized components arising from collisionally populated states. The decay signal of time-resolved fluorescence from 1(1) sigmau+ (nu'=2)]-->1(1) sigmag+(nu"=0) transition was monitored. In the early period after excitation, only very little population in states v'= 1 or 3 had yet accumulated, the rate of collisional activation to the state nu'=2 was negligible. The decay curve of the nu' = 2-->nu" = 0 was treated as a single exponential function. From the measurement of the time-resolved fluorescence, the semilog plot was shown. The slope yielded the effective lifetime of the nu' = 2--> nu' = 0 transition. Based on the Stern-Volmer equation, the radiative lifetime (36 +/- 7) ns was obtained. The total cross sections for deactivation of 1(1) sigmau1 (nu'=2) state by means of collisions with He and H2 are (3.0 +/- 0.5) x 10(-16) cm2 and (6.4 +/- 1.2) x 10(-15) cm2, respectively. The radiative lifetimes of 1(1) sigmau+(nu' = 1,3) states can also be determined through time-resolved fluorescence in pure K vapor. The time-integrated intensities of 1(1)sigmau+(nu' = 1,2,3)-->1(1) sigmag+(nu"=0) transition at different He or Hz pressure were measured. The ratio of fluorescence intensities versus 1/P(He, H2) can be fitted by a straight line. The slopes yield the cross sections sigma(nu'=2-->nu'=1) = (1.4 +/- 0.5) x 10(-16) cm2 and (3.2 +/- 1.0) x 10(-15) cm2; sigma(nu'=2-->nu'=3)= (1.2 +/- 0.4) x 10(-16) cm2 and (2.6 +/- 0.9) x 10(-15) cm2 for He and H2, respectively. Cross sections for the effective quenching of the nu' = 1,2,3 states were also determined. To our knowledge, the cross-sections for these processes are reported for first time.     

气源分子束外延生长的InPBi薄膜材料中的深能级中心

利用深能级瞬态谱(DLTS)研究了气源分子束外延(GSMBE)生长的InP1-xBix材料中深能级中心的性质。在未有意掺杂的InP中测量到一个多数载流子深能级中心E1,E1的能级位置为Ec-0.38 e V,俘获截面为1.87×10~(-15)cm~2。在未有意掺杂的InP0.9751Bi0.0249中测量到一个少数载流子深能级中心H1,H1的能级位置为Ev+0.31 eV,俘获截面为2.87×10~(-17)cm~2。深中心E1应该起源于本征反位缺陷PIn,深中心H1可能来源于形成的Bi原子对或者更复杂的与Bi相关的团簇。明确这些缺陷的起源对于InPBi材料在器件应用方面具有重要的意义。     

An analysis of pulse propagation through a saturable absorber having excited-state absorption

The theoretical study of the propagation of a bell-shaped light pulse through a saturable absorber having excited-state absorption is presented. Assuming that the pulse-width is longer than the first excited-state lifetime of the absorber, a general expression for the steady-state transmission of the absorber is obtained. It is shown that when the excited-state absorption cross-section is larger than the ground-state absorption cross-section (reverse saturable absorber) the absorber acts as a power limiter. An explicit expression for the change of temporal pulse-width in a single transit through the absorber is obtained, which shows that the pulse-width increases due to the presence of excited-state absorption. An analytical expression is presented for the optimum pulse intensity at which the maximum pulse broadening occurs.