Field-free molecular orientation enhanced by tuning the intensity ratio of a three-color laser field

We theoretically study the field-free molecular orientation induced by a three-color laser field. The three-color laser field with a large asymmetric degree can effectively enhance the molecular orientation. In particular, when the intensity ratio of the three-color laser field is tuned to a proper value of I_3: I_2: I_1= 0.09 : 0.5 : 1, the molecular orientation can be improved by ～ 20% compared with that of the two-color laser field at intensity ratio I_2: I_1= 1 : 1 for the same total laser intensity of 2×10~(13)W/cm~2. Moreover, we investigate the effect of the carrier-envelope phase(CEP) on the molecular orientation and use the asymmetric degree of the laser field to explain the result. We also show the influences of the laser intensity, rotational temperature, and pulse duration on the molecular orientation. These results are meaningful for the theoretical and experimental studies on the molecular orientation.     

Studies on the mechanisms of powerful terahertz radiations from laser plasmas

A survey on the mechanisms of powerful terahertz (THz) radiation from laser plasmas is presented.Firstly,an analytical model is described,showing that a transverse net current formed in a plasma can be converted into THz radiations at the plasma oscillation frequency.This theory is applied to explain THz generation in a gas driven by two-color laser pulses.It is also applied to THz generation in a tenuous plasma driven by a chirped laser pulse,a few-cycle laser pulse,a DC/AC bias electric field.These are well verified by particle-in-cell simulations,demonstrating that THz radiations produced in these approaches are nearly single-cycles and linear polarized.In the chirped laser scheme and the few-cycle laser scheme,THz radiations with the peak field strength of tens of MV/cm and the peak power of gigawatt can be achieved with the incident laser intensity less than 10 17 W/cm 2.     

The dependence on optical energy of terahertz emission from air plasma induced by two-color femtosecond laser-pulses

The generation of terahertz （THz） emission from air plasma induced by two-color femtosecond laser pulses is studied on the basis of a transient photocurrent model. While the gas is ionized by the two-color femtosecond laser-pulses com- posed of the fundamental and its second harmonic, a non-vanishing directional photoelectron current emerges, radiating a THz electromagnetic pulse. The gas ionization processes at three different laser-pulse energies are simulated, and the corresponding THz waveforms and spectra are plotted. The results demonstrate that, by keeping the laser-pulse width and the relative phase between two pulses invariant when the laser energy is at a moderate value, the emitted THz fields are significantly enhanced with a near-linear dependence on the optical energy.     

THz Radiation Generation via the Interaction of Ultra‐short Laser Pulses with the Molecular Hydrogen Plasma

In this paper, a two dimensional Particle In Cell‐Monte Carlo Collision simulation scheme is used to examine the THz generation via the interaction of high intensity ultra‐short laser pulses with an underdense molecular hydrogen plasma slab. The influences of plasma density, laser pulse duration and its intensity on the induced plasma current density and the subsequent effects on the generated THz signal characteristics are studied. It is observed that the induced current density in the plasma medium and THz spectral intensity are increased at the higher laser pulse intensities, laser pulse durations and plasma densities. Moreover, the generated THz electric field amplitude is reduced at the higher laser pulse durations. A wider frequency range for the generated THz signal is shown at the lower laser pulse durations and higher plasma densities. Additionally, it is found that the induced current density in hydrogen plasma medium is the dominant factor influencing the generation of THz pulse radiation. (© 2016 WILEY‐VCH Verlag GmbH & Co. KGaA, Weinheim)     

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.     

Molecular orientation and alignment by intense single-cycle THz pulses

Intense single-cycle THz pulses resonantly interacting with molecular rotations are shown to induce field-free orientation and alignment under ambient conditions. We calculate and measure the degree of both orientation and alignment induced by the THz field in an OCS gas sample, and correlate between the two observables. The data presents the first observation of THz-induced molecular alignment in the gas phase.     

Dynamical analysis of the effect of elliptically polarized laser pulses on molecular alignment and orientation

In this Letter, we study the molecular alignment and orientation driven by two elliptically polarized laser pulses.It is shown that the field-free molecular alignment can be achieved in a three-dimensional(3D) case, while the field-free molecular orientation is only along the x and y directions, and that the field-free alignment and orientation along different axes are related to the populations of the rotational states. It is demonstrated that changing the elliptic parameter is efficient for controlling both in-pulse and post-pulse molecular alignment and orientation. The delay time also has an influence on the field-free molecular alignment and orientation.     

基于光场离化电流机制产生强太赫兹辐射的参数优化研究

基于超短激光脉冲与气体作用通过光场离化电流产生太赫兹(THz)辐射的模型, 研究了用双色激光脉冲的方法产生强THz辐射的优化参数条件. 数值计算表明, 导致THz辐射产生的离化电流主要是由一阶电离过程产生的, 高阶离化对该电流产生的贡献很小. 通过调节基频光与倍频光的配比、相位差都能增大离化电流, 从而可以提高THz辐射振幅. 将激光波长拓展到中红外波段, 也有利于提高离化电流. 此外,改变作用气体的种类也能改变离化电流. 在激光和密度参数相等的情况下, 在氦气中可以产生高于氮气中2倍左右的离化电流.     

Alignment-dependent strong field ionization of molecules

We demonstrate a method to measure strong field laser ionization of aligned molecules. The method employs a macroscopic field-free dynamic alignment, which occurs during revivals of rotational wave packets produced by a femtosecond laser pulse. We investigate the dependence of strong field ionization of N2 on molecular orientation. We determine that N2 molecules are four times more likely to ionize when aligned parallel to the field than when aligned perpendicular to it.     

多脉冲激光增强太赫兹辐射的PIC模拟

 模拟了强激光和稀薄非均匀等离子体相互作用在界面辐射超强太赫兹波的物理过程,提出了利用多脉冲激光增强太赫兹辐射的方案,详细研究了多脉冲激光的脉冲个数（取１～４个）、脉冲间距等因素对太赫兹辐射功率和频率的影响。当入射激光包含4个脉冲时,辐射最强,此时的辐射功率是相同条件下单脉冲的6倍,可达到7.16 MW,辐射的太赫兹波的脉宽约为330 fs,总能量约为1 μJ。研究结果表明:多脉冲激光可以显著增强太赫兹辐射,且随着脉冲个数的增加,激起的电子静电波振幅变大,辐射功率也随之变大,直到尾流场饱和;当脉冲间距等于入射激光脉宽时辐射最强。     

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.     

气体辐射太赫兹波产额与驱动激光强度的依赖关系

利用光电流模型研究了气体辐射太赫兹波产额与驱动激光峰值强度的依赖关系.模拟表明,无论是单色激光脉冲还是双色激光场,当激光较弱时,太赫兹产额随着激光强度的增加而迅速增大;而当气体电离接近或达到饱和后,进一步增强激光场强度,太赫兹产额出现了振荡变化.与通常采用较弱激光强度相比,更高的激光强度(致使气体达到完全电离)会进一步增强太赫兹波的辐射强度.分析各个电离事件所产生电子的个数和运动轨迹的对称性,可以很好地解释这些结果.     

Dramatic Spectral Broadening of Ultrafast Laser Pulses in Molecular Nitrogen Ions

We investigate nonlinear interaction of nitrogen molecules with a two-color laser field composed by an intense800 nm laser pulse and a weak 400 nm laser pulse.It is demonstrated that the spectrum of 400 nm pulses is dramatically broadened when the two beams temporally overlap.In comparison,the spectral broadening in argon is less pronounced,although argon atoms and nitrogen molecules have comparable ionization potentials.We reveal that the dramatic spectral broadening originates from the greatly enhanced nonlinear optical effects in the near-resonant condition of interaction between the 400 nm pulses and the nitrogen molecular ions.     

Coherent control of rotational wave-packet dynamics via fractional revivals

We show (i) how the evolution of a wave packet created from an initial thermal ensemble can be controlled by manipulating interferences during the wave packet's fractional revivals and (ii) how the wave-packet evolution can be mapped onto the dynamics of a few-state system, where the number of states is determined by the amount of information one wants to track about the wave packet in the phase space. We illustrate our approach by (i) switching off and on field-free molecular axis alignment induced by a strong laser pulse and (ii) converting alignment into field-free orientation, starting with rotationally cold or hot systems.     

激光参数影响太赫兹辐射的数值模拟

 利用2维PIC程序模拟了聚焦激光脉冲垂直入射非均匀等离子体,在界面激发超强太赫兹辐射的物理过程,研究了激光强度、脉宽和焦斑半径对太赫兹辐射功率和频率的影响,并和模式转换理论作了对比。结果表明:激光强度是影响太赫兹辐射功率的主要因素;当脉宽在等离子体波长附近时,激起的静电波振幅最大,此时对应的太赫兹辐射最强;同时存在一个最优的焦斑半径,使得辐射功率最大。     

激光等离子体光丝中太赫兹频谱的调控

研究了双色激光场激发空气成丝产生太赫兹辐射频谱的变化规律.实验观察到随驱动光功率和光丝长度增加,太赫兹光谱主要发生红移的现象.分析表明,由于等离子体密度的增加,太赫兹辐射的趋肤深度减小,等离子体吸收主导了红移的发生.在光丝足够短的条件下,趋肤深度远大于光丝长度,从而产生等离子体振荡主导的太赫兹辐射光谱蓝移.本研究为超快宽带太赫兹辐射的频谱调控提供了新思路.     

Four-wave mixing model solutions for polarization control of terahertz pulse generated by a two-color laser field in air

A four-wave mixing （FWM） model is used to analyze the polarization control of terahertz （THz） pulse generated by a two-color laser field in air. The analytic formula for the THz intensity varying with the THz polarizer angle, and the relative phase between the two pulses, are obtained. The corresponding numerical results agree well with both numerical result obtained from a quantum model and measured data reported. Moreover, possible phenomena are predicted for variables not found in other experiments. Compared with the quantum model, the FWM model gives analytic formulas and clear physical pictures, and has the advantage of efficient computing time.     

激光等离子体太赫兹辐射源的频率控制

实验研究了双色超快强激光场作用于氮气分子束所产生的宽带太赫兹(THz)辐射光谱随等离子体介质的密度和长度的依赖关系, 发现THz辐射的中心频率随等离子体密度提高和长度减小而增大(0.8-1.4 THz), 且谱宽也随之增加(0.78-1.53 THz). 分析和计算表明, 太赫兹光谱的变化由等离子体振荡频率和谱宽决定. 该发现为等离子体宽带太赫兹辐射源的光谱操控提供了新思路.     

Theoretical investigation of tunable polarized broadband terahertz radiation from magnetized gas plasma

The mechanism of terahertz(THz) pulse generation with a static magnetic field imposed on a gas plasma is theoretically investigated. The investigation demonstrates that the static magnetic field alters the electron motion during the optical field ionization of gas, leading to a two-dimensional asymmetric acceleration process of the ionized electrons. Simulation results reveal that elliptically or circularly polarized broadband THz radiation can be generated with an external static magnetic field imposed along the propagation direction of the two-color laser. The polarization of the THz radiation can be tuned by the strength of the external static magnetic field.     

Role of highest occupied molecular orbitals in molecular field-free alignment by a femtosecond pulse

This paper studies the molecular rotational excitation and field-free spatial alignment in a nonresonant intense laser field numerically and analytically by using the time-dependent Schr?dinger equation. The broad rotational wave packets excited by the femtosecond pulse are defined in conjugate angle space, and their coefficients are obtained by solving a set of coupled linear equations. Both single molecule orientation angles and an ensemble of O₂ and CO molecule angular distributions are calculated in detail. The numerical results show that, for single molecule highest occupied molecular orbital (HOMO) symmetry σ tends to have a molecular orientation along the laser polarization direction and the permanent dipole moment diminishes the mean of the orientation angles; for an ensemble of molecules, angular distributions provide more complex and additional information at times where there are no revivals in the single molecule plot. In particular, at the revival peak instant, with the increase of temperature of the molecular ensemble, the anisotropic angular distributions with respect to the laser polarization direction of the π _g orbital gradually transform to the symmetrical distributions regarding the laser polarization vector and for two HOMO configurations angular distributions of all directions are confined within a smaller angle when the temperature of the molecular ensemble is higher.