飞秒时间分辨实验中泵浦-探测交叉相关函数的测量和时间零点的确定

飞秒激光技术的出现使得实时探测与跟踪激发态超快弛豫动力学过程成为可能,并能够给出激发态动力学过程清晰的物理图像。而在飞秒时间分辨实验中,泵浦-探测相关函数和时间零点直接影响实验结果的可靠性和准确性。本文结合飞秒激光在分子激发态超快动力学过程中的应用进展,介绍了根据实验条件和要求,在具体实验过程中泵浦-探测相关函数测量和时间零点确定的几种方法。实验中选择可见光作为泵浦光和探测光时,可以通过测定随泵浦-探测时间延迟变化的泵浦激光与探测激光的和频/差频光强来确定泵浦探测交叉相关函数和时间零点;而选择中心波长在紫外甚至真空紫外的激光脉冲作为泵浦光或探测光时,泵浦-探测交叉相关函数通常采用校正的方法测量。     

飞秒激光脉冲整形技术及其应用

通过频域上控制飞秒激光脉冲幅度、相位和偏振在时域上可以获得几乎任意形状的飞秒激光脉冲,这种飞秒激光脉冲整形技术可为研究光与原子分子非线性相互作用提供一种全新实验技术手段.本文介绍飞秒激光脉冲整形发展历史、技术方法、控制方式及其相关应用,并展望飞秒激光脉冲整形技术未来的发展方向.     

调Q激光光折变自适应光外差探测技术研究

基于光折变晶体中自泵浦与互泵浦相位共轭共存效应,利用新型光折变自适应光外差探测系统进行了调Q脉冲激光的光折变自适应光外差探测技术研究.结果表明,该系统可以用来实现单纵模调Q脉冲激光的自适应光外差探测,并可以通过提高本振光强度有效地提高外差探测灵敏度.进一步的实验和理论分析表明,对于一般的调Q脉冲激光,由于其各个纵模频谱分量之间不相关,难于实现光外差探测.     

铋纳米薄膜相干光学声子研究

利用共轴双色飞秒激光泵浦-探测技术测量了铋(Bi)纳米薄膜的相干光学声子。采用自相关技术测量得到探测光的脉宽约为45 fs,用探测光和泵浦光的互相关信号得到泵浦光经过脉冲整形以后的脉宽约为250 fs,进而测量得到Bi纳米薄膜的对称振动模频率为2.86 THz,与自发Raman光谱的结果吻合。采用指数衰减函数与互相关信号的卷积拟合延迟时间在10 ps以内的差分反射信号,确定了相干光学声子振幅衰减的特征时间约为2.6 ps,与电子衰减特征时间相近,却远小于晶格加热的特征时间,从而为进一步揭示材料内部载流子与声子的相互作用提供了依据。     

高重频硬X射线自由电子激光脉冲到达时间诊断方法研究

X射线自由电子激光(XFEL)脉冲时间诊断技术常用于实验站附近XFEL脉冲和配套激光的相对到达时间探测,是飞秒级XFEL泵浦探测实验的重要辅助技术,为XFEL和激光泵浦探测实验中两种脉冲对准提供参考信号.随着XFEL向高重频、短脉冲发展,对时间诊断中的诊断频率、泵浦样品和分辨率提出了更高的要求.该技术通过泵浦探测和光学互相关实现,当XFEL脉冲入射高带宽半导体样品瞬间,导致样品复折射率突变,使XFEL到达时间编码于突变空间.本文基于空间编码和光谱编码两种方法,研发设计了XFEL单脉冲到达时间诊断装置;并通过Beer’s吸收理论和原子散射理论对X射线与样品作用过程进行模拟,研究了该过程中X射线吸收与折射率突变的响应程度,完善了样品的分析选择模型;对光谱编码中的啁啾脉冲调制进行分析,得到色散介质和脉冲本征参数对诊断分辨率的影响.该研究对XFEL脉冲到达时间诊断装置的应用具有指导意义.     

飞秒激光参数对非绝热耦合分子态布居的影响

利用含时波包法研究强飞秒泵浦-探测激光场中激光脉宽、波长和场强对非绝热耦合NaI分子各态布居的影响.波包在势能面上做周期性运动,周期约为1 000 fs.延时为200 fs时,波包第一次到达交叉区域分裂成两部分.波包在交叉区域的分裂情况影响各态布居.脉宽增长,NaI分子的激发概率增大,而解离概率减小.泵浦波长为共振波长318 nm时,激发概率最大.泵浦波长增长,NaI分子的解离概率减小.泵浦场强增大,激发概率增大,但解离概率不变.探测激光波长和场强不影响NaI分子各态布居分布.调节激光场参数可实现对波包运动的控制从而控制态布居的选择性分布.研究结果为实验上实现分子的光控制过程提供参考.     

NaLi分子飞秒含时光电子能谱的理论研究

运用三态模型和含时波包方法,研究了NaLi分子处于强飞秒抽运-探测激光场中的波包动力学过程和时间分辨光电子能谱,并且揭示了飞秒激光脉冲参数与NaLi分子光电子能谱之间的关系.研究发现:对于不同的激光波长,波包的振动周期是不同的,而且随着抽运-探测脉冲延迟时间的不同,NaLi分子光电子能谱的谱峰高度和位置发生变化;当λ1=352 nm并且?t=400 fs时,外阱中相应的光电离信号(0.5 eV处)明显强于内阱中相应的光电离信号(1.35 eV处).计算结果表明,NaLi分子激发态41Σ+上波包动力学的一些信息能够通过其光电子能谱反映出来.这些结果可以为实验上实现分子的光控制以及量子操控过程提供一些有价值的参考信息,并为进一步的理论研究提供重要依据.     

基于液晶空间光调制器的太赫兹波频谱调制

频谱可调制的太赫兹波具有广泛的应用价值。利用一台纯相位式的液晶空间光调制器对飞秒激光脉冲进行空间整形,通过改变飞秒激光脉冲的横向空间分布,实现太赫兹波频谱的调制。在实验中,利用光泵浦整流方式产生太赫兹波,并利用太赫兹时域光谱系统对太赫兹信号进行探测。通过GS算法在液晶空间光调制器上加载不同的相位图,获得了不同的飞秒激光脉冲横向空间分布。通过改变探测距离和飞秒脉冲的空间分布参数,实现了太赫兹波频谱的调制。还利用菲涅尔衍射算法对这一过程进行了理论模拟,理论模拟结果与实验结果吻合的较好,这充分说明了基于飞秒脉冲空间整形的太赫兹光谱调制技术的可行性。     

飞秒激光成丝过程中由等离子体光栅引起的超连续谱增强与转移

在飞秒宽带激光脉冲成丝过程中, 由于双光束干涉效应而形成的空间等离子体光栅, 研究了空气中飞秒宽带激光脉冲成丝所产生的超连续谱增强效应, 并进一步观测到泵浦光脉冲成丝产生的超连续谱能量向较弱的未成丝的探测光脉冲转移, 有效拓展探测光脉冲带宽的新现象. 通过基于布拉格衍射特性的理论计算较好地解释了实验结果.     

自相关法测量飞秒激光双脉冲若干参量的研究

飞秒激光双脉冲在研究光泵浦的超快瞬态过程领域具有重要的应用价值,如何实现高准确度的飞秒激光双脉冲的实时测量显得尤为重要.本文提出了一种基于自相关法的飞秒激光双脉冲参量的测量方法,可实现对共光路传输、具有飞秒至皮秒级时间间隔的飞秒激光双脉冲的脉冲间隔、脉冲宽度和强度比的实时测量.实验中采用自相关仪测得了双折射晶体(钒酸钇)分束出的飞秒激光双脉冲的自相关曲线,并用非线性拟合算法求得了飞秒激光双脉冲的脉冲间隔、脉冲宽度和强度比参量.实验结果表明,本文方法与互相关测量方法相比,克服了参考脉冲参量的不确定性对检测准确度的影响,使测量平均准确度提高了48%以上.     

Optical second harmonic generation and its photoinduced dynamics in ferroelectric semiconductor Sn<Subscript>2</Subscript>P<Subscript>2</Subscript>S<Subscript>6</Subscript>

By means of optical pump–probe technique, the ultrafast dynamics of nonlinear optical response of the ferroelectric semiconductor Sn₂P₂S₆ crystal excited with a femtosecond laser pulse has been investigated. It has been shown that, under the action of femtosecond pulses, change in optical second harmonic generation occurs in the sample, which can be due to screening of existing electric polarization.     

Efficient generation of third harmonic radiation in air filaments: A revisit

In this paper we revisit the third harmonic generation from a femtosecond laser filament in air and its significant enhancement (~ 100 times) with a intercepting pump pulse, which has been reported very recently. The enhanced third harmonic is studied as a function of the pulse polarization, time delay between the pump and signal pulses, laser pulse energy, etc. We provide an explanation for the enhancement of third harmonic based on a quenching of interference effects present near filamentation threshold. Simulations based on a two-color propagation code reproduce well the experimental observations and confirm our interpretation.     

飞秒激光脉冲的谐波频率分辨光学开关法测量研究

建立了一台谐波频率分辨光学开关法(FROG)飞秒脉冲测量装置，利用该装置进行了掺钛蓝宝石飞秒激光脉冲的测量研究.在二次谐波自相关测得的时域和频域信号基础上，结合对信号光强度分布的计算机迭代处理，得到了有关飞秒激光电场、光谱及其相位的信息，所得脉宽与干涉测量的结果基本一致. 关键词： 频率分辨光学开关法(FROG) 迭代计算 飞秒激光 自相关     

The analysis of excite and probe measurements of relaxation times with fluctuating pulse duration

The effect of fluctuations in the pulse duration of synchronously pumped modelocked pulse trains on excite and probe measurements is discussed. Relaxation times comparable with the pulse durations can be measured even when large pulse-to-pulse fluctuations in duration exist. The pump and probe pulse durations are assumed to be correlated. When the probe pulses are the second harmonic of the pump, or vice versa, the third harmonic must also be generated to permit deconvolution of experimental excite and probe data. When the pump and probe pulses have the same time dependence, the excite and probe curves consist of the desired response function convolved with the time-averaged second harmonic autocorrelation function which is easily measured. Deconvolution yields the relaxation time but fluctuations in pulse duration increase the root-mean-square voltage fluctuation at the output of the detector system and limit the accuracy with which the relaxation time can be calculated.     

Time-frequency characterization of high-order harmonic pulses

We present energy-resolved cross-correlation measurements of extreme ultraviolet (XUV) pulses generated as high harmonics of femtosecond pulses from a 1 kHz titanium-sapphire laser. The harmonic pulses are probed by a fraction of the fundamental laser pulse at 800 nm, in a noncollinear geometry, allowing us to vary independently the parameters of the harmonic pump and near-infrared probe pulses. We measure the so-called sidebands in the photoelectron spectrum of argon corresponding to the absorption of a harmonic photon plus or minus one probe photon. Spectrally resolving the cross-correlation signal allows us to characterize the time-dependent frequency of the XUV pulse.Received: 20 December 2002, Published online: 24 April 2003PACS: 42.65.Ky Harmonic generation, frequency conversion     

BBO晶体中飞秒脉冲的二次和三次谐波振荡产生

同时考察了群速色散失配、最低阶群速色散和二阶群速色散。研究了在ＢＢＯ晶体中飞秒激光脉冲的谐产生，计算了ＢＢＯ晶体的作为波长函数的晶体的最低阶和二谐群速色散，借助求解改进的耦合波方程的数值计算，得到了飞秒脉冲的二次及三次谐波辐射，分析了最低工阶及二阶ＧＶＤ对于基波脉冲和谐波脉的影响，最后考虑了三次谐波产生中群速失配的补偿。     

Generation of double pulses in-line by using reflective Dammann gratings

Doubled femtosecond laser pulses in-line are needed in the collinear pump-probe technique, collinear second harmonic generation frequency-resolved optical gating (SHG FROG) and the spectral phase interferometry for direct electric-field reconstruction (SPIDER), etc. Normally, it is generated by using a Michelson's structure. In this paper, we proposed a novel structure with two-layered reflective Dammann gratings and the reflective mirrors to generate doubled femtosecond laser pulses in line without transmission optical elements. Angular dispersion and spectral spatial walk-off are both compensated. In addition, this structure can also compress the positive chirped pulse, which cannot be realized with a Michelson's structure. By adopting triangular grating and blazed gratings, the efficiency of the system would in principle be increased as the Michelson's scheme. Experiments demonstrated that this method should be an alternative approach for generation of the double compressed pulses of femtosecond laser for practical applications.     

利用三色组合脉冲激光获得孤立阿秒脉冲发射

孤立阿秒脉冲因可以跟踪和控制原子及分子内电子的运动过程而备受关注.本文从理论上开展了氦原子在3束飞秒脉冲激光组合场辐照下产生的高次谐波和阿秒脉冲辐射的研究.组合激光场由16 fs/1600 nm,15 fs/1100 nm和5.3 fs/800 nm的钛宝石脉冲构成.与前两束脉冲合成的双色场产生谐波谱相比,附加钛宝石脉冲的三色场产生的高次谐波发射谱呈现出高转换效率及宽带超连续特性,超连续谱范围覆盖从230—690次谐波,傅里叶变换后实现了128 as高强度孤立短脉冲的产生.该结果归因于合成的三色场呈现出高功率及少周期的中红外飞秒脉冲激光特性,可以有效控制原子电离以及复合发生在中红外飞秒脉冲的一个有效光学周期内.     

Spectral modulation and supercontinuum generation assisted by infrared femtosecond plasma grating

Spectral modulation and supercontinuum generation of a probe pulse is investigated by using the plasma grating induced by the interference of two infrared femtosecond laser pulses. The dependences of the supercontinuum generation from the probe pulse on the time delay, the relative polarization angle between the probe pulse and the two-pump pulses, and the input probe pulse energy are investigated. The far-field spatial profiles of the three pulses are measured with different time delays and relative polarization angle, and the core energy of the probe pulse as functions of the time delay and relative polarization angle are also shown.