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。     

基于多光子脉冲内干涉相位扫描法对飞秒激光脉冲进行相位测量和补偿的研究

研制了一套基于多光子脉冲内干涉相位扫描方法的可以同时对飞秒激光脉冲进行相位测量和补偿的实验系统装置.实验中,通过自主研发的LabVIEW程序控制液晶空间光调制器和光纤光谱仪,对待测飞秒激光脉冲施加相位扫描,并同时记录受到调制的飞秒激光脉冲的倍频光谱,得到了多光子脉冲内干涉相位扫描(MIIPS)轨迹图.通过MIIPS轨迹图的三次测量和迭代运算,还原出了经过预先啁啾调制的中心波长约为810 nm、重复频率为1 kHz的飞秒激光脉冲的光谱相位,测量精度在0.1 rad以内.根据测量结果,利用液晶空间光调制器对该飞秒激光脉冲进行相位补偿,得到了近似傅里叶变换极限的飞秒激光脉冲.这一装置将在多光子显微成像、脉冲整形、飞秒激光光谱学等众多领域发挥重要作用.     

不同波长飞秒脉冲的相位测量

飞秒脉冲技术的不断发展能够较方便地产生不同波段和结构特性的飞秒脉冲. 对已有的改进型零附加相位光谱相位相干电场重构系统进行优化整合,使之胜任不同特性飞秒脉冲的测量. 利用该系统测量了两台飞秒激光系统输出不同波长的脉冲及其通过厚度为80 mm的BK7玻璃块而得到的啁啾脉冲. 实验结果表明,该系统的适用范围较宽. 关键词： 光谱相位相干直接电场重构法 飞秒脉冲测量 波长     

罗丹明B溶液中双光子荧光的相干控制

本文利用飞秒激光频谱相位整形技术和偏振调制技术,对罗丹明B溶液中双光子荧光的相干控制进行了研究。通过对飞秒激光脉冲进行π相位扫描和余弦相位调制,实现了罗丹明B溶液中双光子荧光的相干控制,荧光强度能够被有效操控。经过理论模拟与分析,证实罗丹明B溶液中双光子荧光强度的变化由双光子跃迁过程中不同量子路径之间的干涉相长和干涉相消引起的。对激光脉冲进行偏振调制的实验,罗丹明B溶液中双光子荧光强度呈现出周期性变化;经过理论模拟计算,发现这种变化是受激光偏振的影响产生的。     

强光场下非共振双光子跃迁相干控制

利用飞秒激光脉冲相位整形技术,从理论和实验两方面,对强激光场下分子体系苝溶液中非共振双光子跃迁的相干控制进行了研究。通过对飞秒激光脉冲进行相位扫描和余弦相位调制,发现分子体系中非共振双光子的跃迁几率能够被削弱,但不能完全消除。分子体系中非共振双光子跃迁的相干控制受到激光光场的形状和分子吸收谱谱宽的影响;与原子体系相比,分子体系中非共振双光子跃迁相干控制的调制效率降低。     

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.     

负啁啾高强度飞秒脉冲在正常色散材料中传输特性研究

利用块状正常色散材料作非线性介质，实验研究了负啁啾强激光飞秒脉冲在正常色散材料的传输过程中，脉冲波形及频谱随入射脉冲能量的变化特性.实验发现，负啁啾脉冲经过材料后激光光谱在被整形和压缩的同时，脉冲宽度也被压缩.实验获得的压缩脉冲宽度短于相等光谱宽度下的双曲正割转换极限脉冲宽度.数值模拟结果显示，在实验条件下模拟结果具有同样的变化特性. 关键词： 飞秒脉冲 自压缩 负啁啾 自聚焦     

基于瞬态光栅频率分辨光学开关装置的阿秒延时相位控制

操控多路激光脉冲之间的相对延时（相对相位）对于亚周期相干合成技术意义重大.当周期量级脉冲之间的相对延时接近数十飞秒时,常见的飞秒脉冲测量手段已无法满足脉冲之间相对相位的精确调控需求.本文基于瞬态光栅频率分辨光学开关装置,精确反演出脉冲之间的相对相位.此方案不仅有助于直接产生亚周期（亚飞秒）脉冲,还可应用于时间隐身学和二维相干光谱学等相关领域.     

V型原子系统中相干布居俘获的相干相位调制研究

在延迟脉冲激光场作用下的V型原子系统中，实现了对相干布居俘获，电磁感应透明的相干相位调制，选择适当的能级其调制频率可以达到飞秒量级.利用数值和解析分析得到了延迟脉冲和叠加态粒子数布居的关系，以及粒子布居受光场相位调制的特点和变化规律.利用这种机理可以实现飞秒量级的量子开关作用. 关键词： 相干相位调制 相干布居俘获 电磁感应透明 量子开关     

锥形镀膜光纤探针中飞秒激光脉冲的传输

采用三维时域有限差分法对飞秒激光脉冲照明下锥形镀膜光纤探针内的光场进行了计算,研究了飞秒脉冲在探针中传输时的时域、频谱和相位特性,并分析了不同锥角和不同长度的探针对这些特性的影响.研究结果发现飞秒脉冲在探针中传输时出现了脉冲展宽、幅值振荡以及频谱分裂等现象,并且利用频谱和相位的变化特性初步解释了脉冲的展宽和脉冲振幅随时间周期性变化等现象. 关键词： 时域有限差分法 飞秒脉冲 光纤探针     

Coherent rotational states: Their formation and detection

In this paper, we describe molecules and nuclei, with energy spectrum close to that of an ideal rotator, and therefore capable of being pushed into a coherent rotational state. The formation of a coherent rotational state is obtained by means of a strong electromagnetic pulse. In the case of a molecule, resort is made to a laser pulse, while for a nucleus use is made of the Coulomb excitation in a heavy-ion collision. The latter is a thought experiment in that the “coherence” period obtained in the evolution of typical observables is out of reach of experimental detection. For the molecular case, the experiment is feasible and has been done.     

Field-free molecular orientation induced by combined femtosecond single- and dual-color laser pulses：The role of delay time and quantum interference

The coherent control of field-free molecular orientation of CO with combined femtosecond single- and dual-color laser pulses has been theoretically studied. The effect of the delay time between the femtosecond single- and dual-color laser pulses is discussed, and the physical mechanism of the enhancement of molecular orientation with pre-alignment of the molecule is investigated. It is found that the basic mechanism is based on the creation of a rotational wave packet by the femtosecond single-color laser pulse. Furthermore, we investigate the interference between multiple rotational excitation pathways following pre-alignment with femtosecond single-color laser pulse. It is shown that such interference can lead to an enhancement of the orientation of CO molecule by a factor of 1.6.     

Stimulated Raman rotational photoacoustic spectroscopy using a quartz tuning fork and femtosecond excitation

Molecular alignment of linear molecules (O₂, N₂, CO₂ and CO) is measured photoacoustically in the gas phase. The rotational excitation is accomplished using a simple femtosecond stimulated Raman excitation scheme, employing two femtosecond pulses with variable delay between the pulses. Molecular alignment is determined directly by measuring the energy dumped into the gas by quartz-enhanced photoacoustic spectroscopy (QEPAS), utilizing a quartz tuning fork as a sensitive photoacoustic transducer. The experimental results demonstrate for the first time the use of a tuning fork for resonant photoacoustic detection of Raman spectra excited by femtosecond double pulses and match both simulation and literature values.     

Controlled rotational Raman echo recurrences and modulation of high-intensity ultrashort laser pulses by molecular rotations in the gas phase

We show that sequences of femtosecond laser pulses can control the rotational Raman response of a gas mixture, giving rise to a tunable manifold of echo recurrences in the retarded nonlinear-optical response of the gas. Tailored phase masks for high-intensity ultrashort laser pulses are experimentally demonstrated using molecular rotations in the gas phase driven by optimally time-ordered pulse sequences.     

Narrow-band coherent anti-stokes Raman signals from broad-band pulses

By tailoring the phase of a 100 femtosecond probe pulse we are able to obtain a narrow-band coherent anti-Stokes Raman spectroscopy (CARS) resonant signal with a width of less than 15 cm(-1), which is an order of magnitude narrower than the CARS signal from a transform limited pulse. Thus, by measuring the spectrum of the CARS signal we are able to obtain a high-resolution energy level diagram of the probed sample in spite of the broad femtosecond pulse spectrum.     

Application of an optical pulse stretcher to coherent anti-Stokes Raman spectroscopy

An external optical cavity pulse stretcher for nanosecond-long laser pulses has been applied to coherent anti-Stokes Raman spectroscopy (CARS). An increased signal-to-noise ratio was achieved for both vibrational and pure rotational CARS, while the power density of the laser beams remained constant. Moreover, it was demonstrated that the use of the pulse stretcher also leads to improved precision of the determined temperatures and concentrations as a result of repeated excitation of the dye laser.     

Theoretical and experimental investigations of coherent phonon dynamics in sapphire crystal using femto- second time-resolved coherent anti-Stokes Raman scattering

We report on the theoretical and the experimental investigations of the coherent phonon dynamics in sapphire crystal using the femtosecond time-resolved coherent anti-Stokes Raman scattering (fs-CARS) technique. The temporal chirped white-light continuum (WLC) is used for the Stokes pulse, therefore we can perform the selective excitation of the phonon modes without using a complicated laser system. The expected quantum beat phenomenon is clearly observed. The theoretical formulas consist very well with the experimental results. The dephasing times of the excited phonon modes, the wavenumber difference, and the phase shift between the simultaneously excited modes are obtained and discussed. This work opens up a way to study directly high-frequency coherent phonon dynamics in bulk crystals on a femtosecond time scale and is especially helpful for understanding the nature of coherent phonons.     

Selective excitation of the molecular rotational wave packet by two time-delayed laser pulses

In this paper, we investigate the control of the molecular wave packet of a linear molecule by two femtosecond laser pulses. It is shown that the odd and the even rotational wave packets created by a single laser pulse can be selectively excited by accurately controlling the time delay of another laser pulse. By inserting the peak of the second laser pulse at the position of maximum or minimum value around quarter or three quarter rotational period of the slope curve with odd (or even) rotational wave packet contribution that is created by the first laser pulse, the odd rotational wave packet can be enhanced (or suppressed) while the even rotational wave packet is suppressed (or enhanced). As a result, the molecular alignments around quarter and three quarter rotational periods can be obtained. Moreover, it is also shown that by inserting the second laser pulse around the quarter or three quarter rotational periods, the changes in the maximum degree of the molecular alignment for the odd and the even rotational wave packet contributions are consistent with their corresponding slope curves at these positions.     

Quantum state reconstruction of a rotational wave packet created by a nonresonant intense femtosecond laser field

We have experimentally determined the amplitudes and phases of a rotational wave packet in an adiabatically cooled benzene molecule, created by a nonresonant intense femtosecond laser field. In this wave-packet reconstruction, the initial wave packet is further interfered by a replica of the first laser pulse, and the resultant modulation in population is observed in a state-resolved manner. Though several states with different nuclear-spin modifications are populated in the initial condition, a single wave packet created from one of them (with J=0) is specifically reconstructed. Phase shifts characteristic of stepwise Raman excitation beyond the perturbative regime are experimentally identified.     

Femtosecond dynamics of primary processes in visual pigment rhodopsin

The dynamics of the coherent photoisomerization of the 11-cis-retinal in bovine rhodopsin is studied by femtosecond time-resolved laser absorption spectroscopy with a resolution of 30 fs. Rhodopsin is excited with 500-, 535-, and 560-nm femtosecond pulses to produce different initial Franck-Condon states with different vibrational energies of the molecule in its electronically excited state. The time evolution of the photoinduced differential absorption spectra of rhodopsin is measured upon excitation with a femtosecond pulse in a spectral range from 400 to 720 nm. Oscillations in the time-resolved absorption of the rhodopsin photoproducts, such as photorhodopsin with a vibrationally excited all-trans-retinal and in its initial-state rhodopsin with a vibrationally excited 11-cis-retinal, are examined. It is demonstrated that these oscillations reflect the dynamics of coherent vibrational wavepackets. The Fourier transform of these oscillatory components yields frequencies, amplitudes, and initial phases of various vibrational modes involved in the motion the wavepackets in both photoproducts. The main vibrational modes manifest themselves at frequencies of 62 and 160 cm^?1 for photorhodopsin and 44 and 142 cm^?1 for initial-state rhodopsin. It is shown that these vibrational modes are directly involved in the coherent reaction under the study, with their amplitudes in the power spectrum produced by the Fourier transform of the kinetic curves being dependent on the wavelength of rhodopsin excitation.