Optimal control of nonadiabatic alignment of rotationally cold N2 molecules with the feedback of degree of alignment

Nonadiabatic alignment of rotationally cold N2 molecules is optimally controlled by shaping femtosecond pump pulses with the feedback of degree of alignment evaluated by an ion imaging technique. The alignment is optimized by doubly peaked pulses with approximately equal intensities. A doubly peaked pulse with an appropriate interval can be regarded as a single pulse with a center trough based on the considerations from both time and frequency domains, suggesting that the effective duration of a doubly peaked pulse rather than its structure is crucial to nonadiabatic molecular alignment.     

Angular distributions of CH3I fragment ions under the irradiation of single pulse and trains of ultrashort laser pulses

The angular distribution of CH₃I is investigated experimentally using a single Fourier transform-limited laser pulse and a pulse train, where a 90-fs 800-nm linearly polarized laser field with a moderate intensity of 2.8×10¹³ W/cm² is used. The dynamic alignment is demonstrated in a single pulse experiment. Moreover, a pulse train is used to optimize the molecular alignment, and the alignment degree is almost identical to that with the single pulse. The results are analysed by using chirped femtosecond laser pulses, and it demonstrates that the structure of pulse train rather than its effective duration is crucial to the molecular alignment.     

Conservation of molecular alignment for cyclic rotational wave packets in periodic pulse trains

The existence of states for which molecular alignment can be maintained for long periods of time is shown. These states, consisting of coherent superpositions of rotational states, are found among cyclic states of the generalized Floquet operator corresponding to a molecule in a short nonresonant laser pulse. For a single pulse alignment can be maintained, in some cases, for more than 40 times the pulse duration. Because of the special properties of these coherent states, arbitrarily long alignment can be achieved by using well-timed pulse trains.     

Measurement of laser-induced alignment of molecules by cross defocusing

The field-free alignment of CO2 produced in response to the excitation of a molecule by a high-intensity femtosecond pump pulse is measured with a simple coronography-like technique. The technique is based on the defocusing of a time-delayed probe pulse produced by the spatial distribution of aligned molecules. In the intensity regime explored here, the technique is shown to give valuable information about dynamic alignment. With the help of simulations, the degree of alignment is extracted from the data.     

Active manipulation of the selective alignment by two laser pulses

This paper solves numerically the full time-dependent Schrdinger equation based on the rigid rotor model, and proposes a novel strategy to determine the optimal time delay of the two laser pulses to manipulate the molecular selective alignment. The results illustrate that the molecular alignment generated by the first pulse can be suppressed or enhanced selectively, the relative populations of even and odd rotational states in the final rotational wave packet can be manipulated selectively by precisely inserting the peak of the second laser pulse at the time when the slope for the alignment parameter by the first laser locates a local maximum for the even rotational states and a local minimum for the odds, and vice versa. The selective alignment can be further optimised by selecting the intensity ratio of the two laser pulses on the condition that the total laser intensity and pulse duration are kept constant.     

Dynamics of molecular alignment steered by a few-cycle terahertz laser pulse

The field-free alignment of molecule ClCN is investigated by using a terahertz few-cycle pulse (THz FCP) based on the time-dependent density matrix theory. It is shown that a high degree of molecular alignment can be obtained by changing the matching number of the THz FCPs in the adiabatic regime and the non-adiabatic regime. The matching number can affect both the maximum value of the alignment and the time at which it is achieved. It is also found that a higher degree of alignment can be achieved by using the THz FCP at lower intensity and there exists an optimal threshold of molecular alignment with the increase of the field amplitude. Also found is the frequency sensitive region in which the degree of maximum alignment can be enhanced greatly by modulating the center frequencies of different THz FCPs. The investigation demonstrates that comparing with a THz single-cycle pulse, a better result of the field-free alignment can be created by a THz FCP at a constant rotational temperature of molecule.     

Experimental observation of revival structures in picosecond laser-induced alignment of I2

We report the experimental observation of revival structures in the alignment of a ground-state rotational wave packet following nonresonant excitation of I2 molecules by an intense picosecond laser pulse. The revivals appear at characteristic time delays following the excitation by the pump laser pulse, and show a significant narrowing of the angular distribution during a few picoseconds. The interaction with the pump laser also leads to a steady-state alignment of the molecule, due to rotational pumping.     

Dynamic Alignment of D2 Enhanced by Two Few-cycle Pulses

利用数值方法求解D2分子刚性转子模型在超短飞秒激光脉冲作用下的薛定谔方程,计算了双原子分子D2在两束固定强度的飞秒激光脉冲作用下,延迟时间对于分子取向的影响.结果表明,只要选取合适的延迟时间,就能很好改善分子取向;保持两束激光强度不变,通过调整两束脉冲的宽度,选择合适的延迟时间能够进一步有效提高D2分子的取向程度.     

Effects of aligning pulse duration on the degree and the slope of nitrogen field-free alignment

Through theoretical analysis,we show how aligning pulse durations affect the degree and the time-rate slope of nitrogen field-free alignment at a fixed pulse intensity.It is found that both the degree and the slope first increase,then saturate,and finally decrease with the increasing pump duration.The optimal durations for the maximum degree and the maximum slope of the alignment are found to be different.Additionally,they are found to mainly depend on the molecular rotational period,and are affected by the temperature and the aligning pump intensities.The mechanism of molecular alignment is also discussed.     

Nonadiabatic alignment of asymmetric top molecules: field-free alignment of iodobenzene

Nonadiabatic laser alignment of an asymmetric top molecule is studied using the combination of a quantum dynamical theory and time-resolved photofragment imaging experiments. In particular, the degree of alignment of iodobenzene, induced by an intense, linearly polarized picosecond laser pulse, is calculated and measured. Pronounced alignment is obtained under field-free conditions.     

Single-shot measurement of revival structures in femtosecond laser-induced alignment of molecules

We present a single-shot detection technique for field-free molecular alignment. The method is based on probing the time-varying birefringence of an aligned sample by use of a chirped probe pulse, thus encoding the dependence of the alignment on time onto the spectral domain. The technique is applied to alignment of O2. The recorded signals are well described by an analytical formula.     

Pulse shaping control of alignment dynamics in N2

Control on the alignment transients of impulsively aligned ensembles of N₂ molecules has been demonstrated by the use of laser pulses shaped by a spatial light modulator. An alignment experiment has been inserted in the feedback loop of an evolutionary algorithm that found optimum pulse shapes for a set of criteria. Optimum pulse shapes for the maximization of total alignment and for the control of certain aspects of the revival structures are given. The physical mechanisms responsible for the control are analysed with the help of single‐parameter control schemes and numerical simulations, which allowed us to explore the low‐temperature region. This approach sheds light on the role played by different control mechanisms for the alignment dynamics of a molecular ensemble. Copyright © 2006 John Wiley & Sons, Ltd.     

控制双激光脉冲的宽度提高N2分子的取向

提出了通过控制双激光脉冲宽度的方法来提高N₂分子取向程度. 利用数值方法求解了N₂分子刚性转子模型在双激光脉冲作用下的薛定谔方程,计算了双原子分子N₂在总强度固定的两束激光脉冲作用下,不同脉冲宽度对于N₂分子取向的影响. 研究结果表明,通过调整两束激光脉冲的宽度,选择合适的延迟时间能够有效提高N₂分子的取向程度. 关键词： 双激光脉冲 分子取向 脉冲宽度     

拼接光栅压缩器的时域特性

在拼接光栅和拼接光栅压缩器的设计中,子光栅调节偏差不可避免,各维偏差与拼接光栅的时间特性之间的关系很关键。通过脉冲压缩理论分析得到各维偏差和聚焦脉冲时间宽度展宽之间的解析关系,从数值计算结果分析,面平行左右偏差对脉冲的时间宽度影响较大,必须控制在21.08μrad内;条纹密度差异对脉冲宽度的影响很显著,相对条纹密度的比值应控制在10-5以内;从消除角色散的角度分析,面平行俯仰偏差和条纹平行度偏差可以相互补偿,条纹密度差异和面平行左右偏差也可以相互补偿。     

光谱分辨条纹相机测量高能啁啾脉冲特性

实验演示了光谱分辩条纹相机法测量高能啁啾脉冲特性，该方法不仅可以用于测量纳秒量级的放大啁啾脉冲，还可以实时监测压缩器的调节.通过实验证实百焦耳PW演示平台输出的百焦耳量级的纳秒啁啾脉冲具有可压缩性.     

Effect of tunneling ionization on dynamic alignment and post-ionization alignment of nitrogen molecules irradiated by different laser intensities

The dynamic alignment and post-ionization alignment of nitrogen molecules are investigated while considering the effect of tunneling ionization. The effects of tunneling ionization on the angular distribution are calculated when the molecules are irradiated by different laser intensities. The results show that laser intensity directly affects the time and extent of dynamic alignment. Furthermore, the extent of post-ionization alignment is not only determined by laser intensity but also affected by the final extent of dynamic alignment. The post-ionization alignment will dominate during the process of molecular (or molecular ion) rotational alignment for femtosecond laser pulse. The time of tunneling ionization is a significant factor to the final ensemble angular distribution of molecular ions when laser intensity is low.     

Control of femtosecond filamentation by field-free revivals of molecular alignment

We show that the filamentation dynamics of a femtosecond laser probe pulse can be readily controlled by properly matching it to the quantum revivals of pre-aligned molecules prepared through impulsive rotational Raman excitation with an advancing ultrashort pump pulse. Several features of the filamentation process including supercontinuum generation, the length of the plasma channel generated in the wake of the filament, the associated secondary radiations and the multiple filamentation pattern are all easily modified by tuning the cross phase modulation induced by the field-free revivals of molecular alignment, through the delay between the pump and the probe pulses. We show that molecular alignment can also be used to generate conical waves with extremely short intensity spike called shocked X-waves and to further tune the frequency of a few-cycle laser pulse in the wake of a self-guided intense filament.     

Investigation of the effect of a variety of pulse errors on spin I=1 quadrupolar alignment echo spectroscopy

We report on an analysis of a well known three-pulse sequence for generating and detecting spin I=1 quadrupolar order when various pulse errors are taken into account. In the situation of a single quadrupolar frequency, such as the case found in a single crystal, we studied the potential leakage of single and/or double quantum coherence when a pulse flip error, finite pulse width effect, RF transient or a resonance offset is present. Our analysis demonstrates that the four-step phase cycling scheme studied is robust in suppressing unwanted double and single quantum coherence as well as Zeeman order that arise from the experimental artifacts, allowing for an unbiased measurement of the quadrupolar alignment relaxation time, T(1Q). This work also reports on distortions in quadrupolar alignment echo spectra in the presence of experimental artifacts in the situation of a powdered sample, by simulation. Using our simulation tool, it is demonstrated that the spectral distortions associated with the pulse artifacts may be minimized, to some extent, by optimally choosing the time between the first two pulses. We highlight experimental results acquired on perdeuterated hexamethylbenzene and polyethylene that demonstrate the efficacy of the phase cycling scheme for suppressing unwanted quantum coherence when measuring T(1Q). It is suggested that one employ two separate pulse sequences when measuring T(1Q) to properly analyze the short time behavior of quadrupolar alignment relaxation data.     

基于远场的拼接光栅压缩池的设计

 利用傅里叶光学方法得到了失调拼接光栅压缩池输出光束的远场振幅表达式，建立了分析拼接光栅的各种误差的理论模型，得到了拼接误差对脉冲的影响是附加相位延迟和角度偏转。在要求远场的一倍衍射极限区域的积分能量分布达到理想情况下的90％的条件下，对于含有口径为40 cm、脉宽为0.1~10 ps脉冲的系统进行分析并分别得到了各种误差的容限。     

Postpulse molecular alignment measured by a weak field polarization technique

We report a direct nonintrusive observation of alignment and planar delocalization of CO2 after an intense linearly polarized femtosecond laser pulse excitation. The effects are measured by a polarization technique involving a perturbative probe that itself does not induce appreciable alignment. We show that this technique allows one to measure a signal proportional to -1/3, with theta the angle between the molecular axis and the laser polarization. Simulations that support this analysis allow one to characterize the experimentally observed alignment and planar delocalization quantitatively.