Field-free three-dimensional alignment of polyatomic molecules

We experimentally demonstrate field-free, three-dimensional alignment (FF3DA) of polyatomic asymmetric top molecules. We achieve FF3DA in sulfur dioxide gas using two time-delayed, orthogonally polarized, nonresonant, femtosecond laser pulses. Our method avoids the use of rotational revivals and is therefore more robust to temperature. The alignment is probed using time-delayed coincidence Coulomb explosion imaging. FF3DA will be important for all molecular imaging, dynamics, or spectroscopy experiments for which random alignment leads to a loss of information.     

Field-free alignment of molecules observed with high-order harmonic generation

High-order harmonic generation is demonstrated to provide a sensitive way for an extensive study of dynamic processes in the field-free alignment of strong-field-induced molecular rotational wave packets. The time-dependent harmonic signal observed from field-free-aligned N2, O2, and CO2 has been found to include two sets of beat frequency for pairs of coherently populated rotational states. One of them is the well-known frequency component characterizing the field-free alignment of molecules, and the other is ascribed to the beat that arises from coherence embedded in the wave packet. We discuss the effect of each frequency component on the revival signal observed with the harmonic generation.     

Molecular alignment by trains of short laser pulses

We show that a dramatic field-free molecular alignment can be achieved after exciting molecules with proper trains of strong ultrashort laser pulses. Optimal two- and three-pulse excitation schemes are defined, providing an efficient and robust molecular alignment. This opens new prospects for various applications requiring macroscopic ensembles of highly aligned molecules.     

Alignment of molecules by strong laser pulses

We review how moderately intense laser fields offer an approach to alignment of molecules [1]. In particular, molecules can be aligned along a given space fixed axis, forced to a plane, or their rotations about all three possible axes can be eliminated by choosing a linearly polarized, a circularly polarized, or an elliptically polarized alignment field, respectively. We show how molecules in the gas phase can be aligned by turning on the laser field either slowly (a few nanoseconds) or fast (a few picoseconds) with respect to the rotational period of the molecules. The role of the intensity of the laser field and the rotational temperature of the molecules is discussed. Before concluding we describe how aligned molecules enables control and selectivity in the interaction between polarized light and molecules.Received: 15 November 2002, Published online: 18 March 2003PACS: 33.15.Bh General molecular conformation and symmetry; stereochemistry - 32.80.Lg Mechanical effects of light on atoms, molecules, and ions - 33.80.Gj Diffuse spectra; predissociation, photodissociation - 33.80.Rv Multiphoton ionization and excitation to highly excited states (e.g. Rydberg states) - 34.50.Lf Chemical reactions, energy disposal, and angular distribution, as studied by atomic and molecular beams     

Observation of enhanced field-free molecular alignment by two laser pulses

We show experimentally that field-free alignment of iodobenzene molecules, induced by a single, intense, linearly polarized 1.4-ps-long laser pulse, can be strongly enhanced by dividing the pulse into two optimally synchronized pulses of the same duration. For a given total energy of the two-pulse sequence the degree of alignment is maximized with an intensity ratio of 1:3 and by sending the second pulse near the time where the alignment created by the first pulse peaks.     

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.     

Numerical study on transmission of multimode laser pulses by dye molecules

A theoretical model and a numerical study of the transmission of multimode laser pulses by malachite green dye are presented. Excited state absorption is taken into account. The transmitted pulses exhibit increased intensity fluctuations moderated by the excited state absorption. Reference is made to recent experimental results.     

Nonsequential double ionization of diatomic molecules by elliptically polarized laser pulses

Using the classical ensemble method, we investigate nonsequential double ionization （NSDI） of diatomic molecules by elliptically polarized laser pulses. The results show that the ellipticity of the laser field has a strong suppression effect on NSDI probabilities both in parallel and perpendicular alignments. The double ionization （DI） channel is commonly dominated by NSDI, and the NSDI channel changes with ellipticity. As ellipticity increases, more and more NSDIs occur through recollision excitation with subsequent field ionization （RESI）. Moreover, like the case of linear polarization, the two electrons involved in NSDI for perpendicularly aligned molecules are more likely to emit into the opposite hemispheres as compared to the case of parallel alignment. Additionally, this alignment effect increases as ellipticity increases.     

Dynamic and geometric alignment of molecules induced by intense laser fields

We present a method to discuss simultaneously the relative importance of molecular dynamic and geometric alignment induced by intense laser fields in theoretical view. This method divides the process of molecular alignment into three steps, which are tightly correlated with that of molecular multielectron dissociative ionization and Coulomb explosion. A fourth-order Runge-Kutta algorithm and a developed counting approach are used to calculate the angular distribution of molecules in the first and second steps of molecular alignment. The last step is described by a field-ionization, Coulomb explosion model. The angular distribution of molecules at the critical distance originated from geometric alignment is obtained by calculating the volume of shells associated with a series of particular angle. The final angular distributions of molecules are obtained by properly weighting the results of three steps. The numerical results of distinguishing between dynamic and geometric alignment for certain conditions are presented and discussed. Our computational results show that the alignment mechanism, which dominates the observed anisotropy of angular distributions of ionic fragments for a given condition, is determined by the dependences of the extent of dynamic and geometric alignment on laser parameters and molecular parameters.     

飞秒强激光场中的原子、分子——非微扰现象研究

文章简要回顾了飞秒强激光场中的原子、分子这一研究领域在近年来所取得的一系列里程碑式的重大发现,包括多光子电离、阈上电离、隧穿电离、越垒电离、非顺序双电离、电离稳定化、高次谐波发射等等非微扰现象.讨论了纯量子理论和纯经典方法在处理该类问题时经常遇到的困难.介绍了作者所在小组为此提出的半经典模型及其在解释强场物理现象时所取得的成果.最后对这一领域在未来几年内的可能发展方向作了简单的评述.     

Field-free orientation of diatomic molecule via the linearly polarized resonant pulses

We propose a scheme to coherently control the field-free orientation of NO molecule whose rotational temperature is above 0 K. It is found that the maximum molecular orientation is affected by two factors: one is the sum of the population of M = 0 rotational states and the other is their distribution, however, their distribution plays a much more significant role in molecular orientation than the sum of their population. By adopting a series of linearly polarized pulses resonant with the rotational states, the distribution of M = 0 rotational states is well rearranged. Though the number of pulses used is small, a relatively high orientation degree can be obtained. This scheme provides a promising approach to the achievement of a good orientation effect.     

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.     

低强度周期量级脉冲驱动排列分子的非次序双电离

本文利用三维经典系综模型研究了低强度周期量级脉冲驱动排列分子的非次序双电离. 结果表明, 电子对的关联特性强烈地依赖于分子的排列方向和激光脉冲的载波包络相位; 垂直分子反关联电子对的比例总是高于平行分子反关联电子对的比例; 当载波包络相位从0到π 逐渐增加时, 反关联电子对的数目先增加再减少; 对于平行分子, 电子对的释放总是以正关联为主; 而垂直分子的主导关联模式则依赖于激光脉冲的载波包络相位, 当载波包络相位为0.3π-0.7π之间时, 电子对以反关联释放为主, 其他相位下以正关联为主. 本文利用分子势能曲线和电子返回能量很好地解释了电子关联特性对分子排列方向和载波包络相位的依赖关系.     

Three dimensional alignment of molecules using elliptically polarized laser fields

We demonstrate, theoretically and experimentally, that an intense, elliptically polarized, nonresonant laser field can simultaneously force all three axes of a molecule to align along given axes fixed in space, thus inhibiting the free rotation in all three Euler angles. Theoretically, the effect is illustrated through time dependent quantum mechanical calculations. Experimentally, 3, 4-dibromothiophene molecules are aligned with a nanosecond laser pulse. The alignment is probed by 2D ion imaging of the fragments from a 20 fs laser pulse induced Coulomb explosion.     

Above threshold Coulomb explosion of molecules in intense laser pulses

We have measured and explained a new mechanism of molecular ionization near the appearance intensity that produces a sequence of peaks in the nuclear kinetic energy spectrum separated by the photon energy. Our interpretation is based on an internally consistent model for the nuclear motion during an intense laser pulse. Within this model, the same concepts and language can be used for both dissociation and ionization, leading to a more unified understanding of the dynamics.     

Internal collision double ionization of molecules driven by co-rotating two-color circularly polarized laser pulses

The double ionization process of molecules driven by co-rotating two-color circularly polarized fields is investigated with a three-dimensional classical ensemble model. Numerical results indicate that a considerable part of the sequential double ionization(DI) events of molecules occur through internal collision double ionization(ICD), and the ICD recollision mechanism is significantly different from that in non-sequential double ionization(NSDI). By analyzing the results of internuclear distan...     

Wave-coupling theory of linear electro-optic effect for ultrashort laser pulses

A wave-coupling theory of linear electro-optic (EO) effect for ultrashort laser pulses has been developed. As one of its applications, the linear EO effect of ultrashort Gaussian pulses propagating in LiNbO₃ crystal is demonstrated, with the intensity lower than the damage threshold. It is found that the EO effect is sensitive to both the azimuth angle and the polar angle of wave vector of light. And the larger the applied electric field, the shorter the crystal used for optimization of EO coupling is. The numerical results show that, with the duration of input pulse changing from 150 fs to 5 fs, the durations of output pulses are broadened due to the group-velocity dispersion, as well as the first- and second-order refractive dispersion. In addition, when input pulse duration is larger than 20 fs, in contrast with zero chirp, the output durations can be slightly compressed if a positive chirp input pulse is used. The validities of slowly varying amplitude approximation and continuous wave approximation are also discussed. The influence of self-phase modulation and cross-phase modulation on the EO effect is also discussed briefly.     

Propagation of few-cycle laser pulses through a linear gas medium

We investigate the ultrashort pulse propagation through a linear gas medium by direct solution of the wave equation beyond the often used lowest orders of the dispersion approximation and the assumption of a slowly varying envelope. The dispersion effects and the effective absorption of the pulse energy by the medium are shown to result in a strong dispersive broadening of the initial pulse in the time and space domains. New features of the polarization response of the medium resulting from essentially nonadiabatic ramps of the pulse envelope are found. The possibility of using the two-pulse experimental scheme to partly compensate for the dispersion is discussed.