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.     

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     

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.     

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.     

Strong-field molecular ionization: determination of ionization probabilities calibrated with field-free alignment

We report an original optical method providing the probability of molecular ionization induced by femtosecond laser pulses. The approach consists of exploiting molecular alignment to extract reliable information about ionization. The cross defocusing technique implemented for this purpose reveals a sensitivity with respect to postpulse alignment, as well as to the free electron density induced by the ultrashort laser pulse. The analysis of the resulting signal thus gives access to absolute single-ionization probabilities calibrated through the degree of alignment, provided that free electrons are produced mainly by single ionization. The relevance of the method is assessed in N2.     

Compression grating alignment by far-field monitoring

Slight non-parallelism of the gratings in the compressor of a chirped-pulse amplification laser system produces angular chirp which results in a significant reduction of the focused intensity due to elongation of the pulse duration and enlargement of the focal spot. The effect of three-dimensional relative misalignment angles between two gratings on the far-field pattern of the pulses propagating through them is investigated by ray tracing. The far-field pattern provides two-dimensional information of the uncompensated angular dispersion directly. A simple and intuitive alignment procedure to achieve parallelism of the compression gratings by far-field monitoring is demonstrated experimentally, while the alignment precision is found to be the same as the methods proposed previously.     

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.     

Field-free molecular alignment and its application

Field-free molecular alignment can be achieved by nonadiabatic rotational excitation of molecules with strong femtosecond laser pulses. We experimentally and theoretically demonstrate that the degree of alignment can be improved with multi-pulse excitation. An approach is proposed to tune the frequency of few-cycle pulses using field-free alignment of molecules.     

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.     

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.     

Field-free three dimensional molecular axis alignment

We investigate strategies for field-free three dimensional molecular axis alignment using strong nonresonant laser fields under experimentally realistic conditions. Using the polarizabilites and rotational constants of an asymmetric top rotor molecule (ethene, C2H4), we consider three different methods for axis alignment of a Boltzmann distribution of rotors at 4 K. Specifically, we compare the use of impulsive kick laser pulses having both linear and elliptical polarization to the use of elliptically polarized switched laser pulses. We show that an enhanced degree of field-free three dimensional alignment of ground vibronic state molecules obtains from the use of two orthogonally polarized, time-separated laser pulses.     

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.     

Comparison of frequency-resolved optical polarization gating induced by molecular alignment and Kerr effects

We experimentally demonstrated that both the electronic Kerr effect and the molecular alignment in gaseous molecules could be applied as transient gates to diagnose 400 nm target pulses. Their birefringence dissimilarity was clearly visualized by the measured spectrogram and retrieved gate function. In the atomic gas argon, a relatively weak and instantaneous cross phase modulation within the pulse duration was observed, while in the molecular gas N(2), the delayed rotational Raman excitation played a dominative role.     

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.     

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.     

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.     

Evolutionary algorithms in the optimization of dynamic molecular alignment

We numerically study the optimization of dynamic molecular alignment by shaped femtosecond pulses. It is found that an accurate synchronization of the applied field to the molecular response is needed to obtain maximum alignment. Simple approaches based on low-dimensional parametrizations of the electric field are shown to be clearly inferior, especially in the strongly nonperturbative regime.     

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.     

Rotational quasienergy states and alignment of molecules in a strong laser field

The interaction of a molecule with a strong laser field is investigated. Raman-type transitions between rotational levels of a fixed vibrational state of the ground-state term are taken into account in the “quantum rotator” approximation. An initial problem of the evolution of the state of a molecule interacting with a pulsed field is solved. The dynamics of the degree of alignment of a molecule with respect to the direction of polarization of the field during the pulse is investigated. It is shown that for sufficiently long pulses with a smooth envelope the axis of the molecule adiabatically follows the time-varying field amplitude, and alignment is maximum when the field intensity is maximum. It is shown that alignment of molecules can be substantial only if the second-order composite matrix elements, determining the probability amplitudes of transitions between rotational levels of a molecule, are much greater than the dissociation broadening of the levels. The angular distribution of the dissociation products of a molecule in a strong laser field is investigated. Zh. éksp. Teor. Fiz. 116, 1551–1564 (November 1999)