Femtosecond holography in lithium niobate crystals

Spatial gratings are recorded holographically by two femtosecond pump pulses at 388 nm in lithium niobate (LiNbO3) crystals and read out by a Bragg-matched, temporally delayed probe pulse at 776 nm. We claim, to our knowledge, the first holographic pump-probe experiments with subpicosecond temporal resolution for LiNbO3. An instantaneous grating that is due mostly to the Kerr effect as well as a long-lasting grating that results mainly from the absorption caused by photoexcited carriers was observed. The Kerr coefficient of LiNbO3 for our experimental conditions, i.e., pumped and probed at different wavelengths, was approximately 1.0 x 10(-5) cm2/GW.     

Measurement of nonlinear absorption coefficients in GaAs, InP and Si by an optical pump THz probe technique

An optical pump terahertz (THz) probe method for measuring carrier mobility and multiphoton absorption coefficients in semiconductors is demonstrated. A THz probe pulse is used to detect the transient photoconductivity generated by an optical pump pulse. The change in transmission coefficient at THz frequencies due to a pump pulse with photon energy greater than the band gap energy is used to determine the sum of electron and hole mobilities. The weak nonlinear absorption of a pump pulse with photon energy less than the band gap energy produces an approximately uniform free carrier distribution. The THz transmission coefficient vs. pump fluence, and the mobility, are used in a bulk photoconductivity model to determine the multiphoton absorption coefficients. For GaAs, InP and Si we find two photon absorption coefficients at 1305 nm of 42.5 ± 11, 70 ± 18 and 3.3 ± 0.9 cm/GW, respectively. For GaAs and InP we determine three photon absorption coefficients at 2144 nm of 0.19 ± 0.07 and 0.22 ± 0.08 cm³/GW².     

Evidence for two-path recombination of photoinduced small polarons in reduced LiNbO(3)

The recombination of photoinduced free Nb(4+)(Nb) and bound Nb(4+)(Li) small polarons toNb(4+)(Li): Nb(4+)(Nb) bipolarons is investigated in nominally pure, reduced LiNbO(3) single crystals by means of excited-state-absorption spectroscopy. We discovered a two-component decay of the light-induced absorption alpha(li)(t) for probe light at lambda=785 nm and moderate pump beam intensities (I(p) < 670 GW/m(2)). These experimental results give strong evidence for the existence of a two-path recombination of the photoinduced polarons. A corresponding model taking into account hopping charge transport and trapping is presented.     

Linear and nonlinear absorption,SHG and photobleaching behaviors of Dy doped GaSe single crystal

The linear absorption, nonlinear absorption (NA), second harmonic generation (SHG) and carrier mobilities of undoped and 0.1 at% Dy doped GaSe single crystals grown by modified Bridgman method have been studied by UV–vis, open aperture Z-scan, SHG and transmission ultrafast pump probe spectroscopy experiments. Both linear absorption and SHG measurements clearly showed that the doping of GaSe crystal with Dy³⁺ leads to a shift in the linear absorption edge. The mechanisms contributing to the NA behavior were explained and discussed. The photobleaching behaviors of the crystals were investigated by delaying of the probe signal in transmission pump-probe spectroscopy experiments.     

双缺陷模一维光子晶体的双光子吸收增强研究

采用真空镀膜工艺制备了具有762 nm和800 nm双缺陷模的含两个CdS缺陷层的TiO2/SiO2一维光子晶体,运用抽运探测技术测量了其双光子吸收。对于两个缺陷模,双光子吸收均得到很大的增强,其中缺陷模为800nm时的双光子吸收系数307 cm/GW要大于缺陷模为762 nm时的116 cm/GW,分别为单层CdS薄膜的48倍和18倍。这种双光子吸收的增强是由于光局域化导致一维光子晶体缺陷层内的电场强度增大而形成的。通过传输矩阵法计算了一维光子晶体的内部场强,发现800 nm波长光入射时缺陷层内的电场强度要大于762 nm波长光入射时的电场强度值。     

Measurement of two-photon absorption using the photo-thermal lens effect

We report on new schemes for pump-probe photo-thermal lens methods aimed for measuring the two-photon absorption coefficient of a given material. We show that by focusing a probe beam in the presence of a nearly collimated pump beam, we create a thermal lens which yields measurement of the two-photon absorption coefficient of nitrobenzene of (3.9 ± 0.3) 10⁻¹⁰ cm/W at 532 nm. We also show that when the pump field is focused in the presence of a nearly collimated probe beam the width of the z-scan signature of a two-photon absorption process is nearly one order of magnitude smaller than that of a one-photon process. We show experimental evidence of the effect obtained for nitrobenzene.     

All-optical display using photoinduced anisotropy in a bacteriorhodopsin film

Photoinduced anisotropy in a bacteriorhodopsin film using the pump-probe method was investigated. A diode-pumped second-harmonic YAG laser was used as the pump beam, and three wavelengths, at lambda = 442, 532, 655 nm, from different lasers were used as probe beams. Without the pump beam, the probe light cannot transmit the analyzer to the detector. However, because of photoinduced anisotropy, a portion of the probe light is detected when the pump beam is present. Based on this property, we demonstrate a full-color all-optical display.     

长寿命吸收过程对超快动力学过程测量的影响

使用飞秒时间分辨抽运-探测透射光谱技术,实验研究了GaAs体材料中光激发载流子的超快弛豫动力学的波长依赖.在相同的光激发载流子浓度和抽运/探测比时,发现760 nm和780 nm两中心波长处的瞬态透射变化延迟扫描信号出现负的和振荡的信号.与模拟计算结果对比,判定该实验瞬态信号是错误的.分析探测器输出波形,发现是由于反相波形导致的,而引起反相波形的原因在于样品中存在长寿命的吸收过程.指出通过提高探测器上的抽运/探测比能够矫正反相波形,从而获得正确的瞬态透射变化动力学.提高探测器上的抽运/探测比与目前的应尽量减小抽运光对探测器的散射贡献的观点是对立的.文章的研究结果对应用抽运-探测时间分辨光谱技术正确地测量超快瞬态动力学过程具有重要的参考价值. 关键词： 时间分辨抽运-探测透射光谱 饱和吸收 吸收增强 GaAs体材料     

Ultrafast tunable filter in two-dimensional organic photonic crystal

A tunable filter made from a two-dimensional polystyrene photonic crystal is fabricated by focused ion-beam etching. The pump and probe scheme is adopted to measure tunability based on the picosecond optical Kerr effect. The response time of the tunable filter, approximately 10 ps, is within the measurement resolution. The maximum shift of optical channels is estimated to be 6 nm under excitation of 15.9 GW/cm2 pump intensity, which is in agreement with the theoretical prediction.     

Femtosecond Kerr ellipsometry in polydiacetylene solutions: Two-photon effects

We describe a pump-probe femtosecond Kerr experiment in polydiacetylene solutions (4BCMU, yellow form). The Kerr ellipsometry technique permits a separate determination of the real and of the imaginary part of anisotropic index changes. The wavelength (620 nm) of the pump pulses lies in the transparency region of polydiacetylene while the probe pulses have a broad white spectrum. The largest contribution to the Kerr signal is a quasi-resonant stimulated anti-Stokes Raman absorption. A flat two-photon transition spectrum with 4×10^–3 cm/MW is observed close to 4 eV. The two-photon excited states have a life time close to 12 ps and they present a broad absorption band in the 2 eV range.     

Two-photon absorption of high-power picosecond pulses in PbWO<Subscript>4</Subscript>, ZnWO<Subscript>4</Subscript>, PbMoO<Subscript>4</Subscript>, and CaMoO<Subscript>4</Subscript> crystals

The nonlinear process of two-photon interband absorption is studied in tungstate and molybdate oxide crystals excited by a sequence of high-power picosecond pulses with a wavelength of 523.5 nm. The transmission of the crystals is measured for the excitation pulse intensity up to 100 GW/cm². The pulse intensity in the crystals initially transparent at a wavelength of 523.5 nm is strongly limited due to two-photon absorption (TPA), and the reciprocal transmission in PbWO₄ and ZnWO₄ crystals reaches 50–60. In all crystals, TPA induces long-lived one-photon absorption, which affects the nonlinear process dynamics and leads to a hysteresis in the dependence of the transmission on the laser excitation intensity. Absorption dichroism manifests itself in a significant difference in the transmission intensities when the principal orthogonal optical axes of the crystals are excited. The TPA coefficients are determined during the excitation of two optical axes of the crystals. TPA coefficients β for the crystals vary over a wide range, namely, from β = 2.4 cm/GW for PbMoO₄ to β = 0.14 cm/GW for CaMoO₄, and the values of β can differ almost threefold when different optical axes of a crystal are excited. Good agreement is achieved between the measured intensities limited by TPA and the estimates calculated from the measured nonlinear coefficients. Stimulated Raman scattering (SRS) upon excitation at a wavelength of 523.5 nm is only detected in two of the four crystals under study. The experimental results make it possible to explain the suppression of SRS by its competition with TPA, and the measured nonlinear coefficients are used to estimate this suppression.     

Modeling and identification on nonlinear saturable and reverse-saturable absorptions of gold nanorods using femtosecond Z-scan technique

An improved Z-scan analysis approach is proposed by establishing and solving the saturable absorption (SA) and reverse-SA (RSA) models, respectively. Near-infrared femtosecond Z-scans are carried out on the synthesized gold nanorods (NRs) possessing the average length of 46 nm using a femtosecond laser operated at the wavelength of 800 nm, which is close to the peak position of longitudinal surface plasmon resonance (SPR) (710 nm) of gold NRs. At lower input intensity of less than 400 GW/cm2 , the normalized transmission exhibits only SA phenomenon; however, when it exceeds 400 GW/cm2 , both SA and RSA are observed. By using the presented Z-scan modeling and theory, the three-photon absorption (3PA) is identified in the material, and the 3PA cross-section is determined to be 1.58×1071 cm6s2 .     

GaSe晶体的双光子吸收对太赫兹输出的影响

根据光整流效应,利用超快激光脉冲泵浦GaSe晶体实现了0.2~2.5 THz的宽带太赫兹辐射输出。禁带中的电子在两个800 nm光子的作用下激发到导带中形成自由载流子,进而吸收所产生的太赫兹辐射,最终导致太赫兹的输出随泵浦功率的增加而趋于饱和。为了研究双光子吸收对太赫兹输出的影响,测量了800 nm处的GaSe晶体的双光子吸收系数,结果为 0.165 cm/GW。通过对太赫兹输出实验数据的拟合,得到GaSe晶体中自由载流子对太赫兹输出的吸收截面为1×10^-15 cm²。本文的研究结果可用于优化GaSe晶体在强激光泵浦下的太赫兹转换效率。     

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.     

泵浦-探测技术中受激量子拍的理论研究

基于V型三级级原子由于真空与原子耦合引起的量子相干效应,研究了泵浦-探测技术中透射受激量子拍特征.理论计算表明:这种受激量子拍与荧光量子拍相比具有高的信噪比.理论结果与实验有较好的一致性.     

Measurements of photoinduced refractive index changes in bacteriorhodopsin films

We report the pump-probe measurements of nonlinear refractive index changes in photochromic bacteriorhodopsin films. The photoinduced absorption is caused by pump beam at 532 nm and the accompanying refractive index changes are studied using a probe beam at 633 nm. The proposed technique is based on a convenient and accurate determination of optical path difference using digital interferometry-based local fringe shift. The results are presented for the wild-type as well as genetically modified D96N variant of the bacteriorhodopsin.      

基于电子自旋弛豫全光开关中的瞬态特性

设计了基于电子自旋弛豫的透射式全光开关模犁.该光开关具有开关时间短、结构简单,光学非线性强等特点.研究在右旋圆偏振光抽运下 GaAs/AlGaAs半导体多量子阱(MQWs)中以相空间填充(PSF)和库仑屏蔽(CS)为主要因素导致的激子吸收饱和行为,计算与抽运光同向(探测光与抽运光的圆偏振方向相同)和反向(探测光与抽运光的圆偏振方向相反)的圆偏振探测光吸收系数的变化,得到两种圆偏振光差分透射率改变量随延迟时间的变化.实验采用飞秒抽运-探测技术,获得了室温下GaAs/AlGaAs多量子阱同向圆偏振探测光的透射曲线,观察到了明显的饱和吸收现象,与数值模拟的结果相符.     

Low-threshold, self-frequency-stabilized AgGaS(2) continuous-wave subharmonic optical parametric oscillator

We report the demonstration of a cw AgGaS(2) optical parametric oscillator (OPO). The subharmonic (3omega ? 2omega + omega) OPO is configured as a doubly resonant oscillator with weak pump enhancement. The temperature-tuned, noncritically phase-matched crystal is pumped by a diode laser at lambda(p) approximately 845 nm . Oscillation at lambda(s) approximately 1267 nm and lambda(i) approximately 2535 nm is observed at an input threshold power of 60 mW. Crystal thermal loading induces a robust passive self-frequency stabilization of any single-axial-mode pair to the OPO cavity resonance. The conversion efficiency is limited by thermal effects to 2% for a 200-mW pump input.     

Integrated optical Ti:Er:LiNbO3 distributed Bragg reflector laser with a fixed photorefractive grating

For the first time to the authors' knowledge, an integrated optical distributed Bragg reflector laser with a fixed photorefractive grating in LiNbO(3) is demonstrated. Sample preparation, grating fabrication, and laser characteristics are reported. The device is pumped by a fiber pigtailed laser diode (lambda(p) approximately 1480 nm) through the Bragg grating in a double-pass configuration, yielding an emission in the backward direction at lambda=1531.7nm . The laser threshold is 40 mW; as much as 5 mW of output power has been obtained at 110 mW of launched pump power in cw operation.     

YbVO4晶体的受激拉曼散射

采用腔外单次通过方式,研究了一种新型晶体YbVO₄的受激拉曼散射.当抽运激光为532 nm皮秒脉冲时获得了3级斯托克斯线(558.47 nm, 587.92 nm, 620.67 nm)和1级反斯托克斯线(507.58 nm),测得YbVO₄晶体1级斯托克斯受激拉曼散射的稳态增益系数为17.8±0.2 cm/GW,受激拉曼散射的整体转换效率达到37%.实现了YbVO₄晶体对355 nm皮秒激光的受激拉曼散射,观察到1级斯托克斯线(366.1 关键词： 受激拉曼散射 稳态增益系数 转换效率 4晶体')" href="#">YbVO₄晶体