Dissociative ionization of molecules in intense laser fields

Accurate and efficient grid based techniques for the solution of the time-dependent Schrödinger equation for few-electron diatomic molecules irradiated by intense, ultrashort laser pulses are described. These are based on hybrid finite-difference, Lagrange mesh techniques. The methods are applied in three scenarios, namely H₂ ⁺ with fixed internuclear separation, H₂ ⁺ with vibrating nuclei and H₂ with fixed internuclear separation and illustrative results presented.Received: 19 November 2002, Published online: 24 April 2003PACS: 02.60.Cb Numerical simulation; solution of equations - 02.70.Bf Finite-difference methods - 33.80.Rv Multiphoton ionization and excitation to highly excited states (e.g., Rydberg states) - 33.80.-b Photon interactions with molecules     

Triple-ionization-induced dissociation of molecules in strong laser fields

We study triple-ionization-induced dissociation in diatomic molecules with different laser polarizations.     

Resonant Auger decay study of core-excited OCS

The present work aims at characterizing short-lived C1s⁽⁻¹⁾π^*(1) core-excited states of the OCS molecule based on the analysis of the vibrational fine structure and lineshape profiles of the high-resolution resonant Auger decay spectra recorded at the excitation energies along the C1s→π^* resonance in the binding energy region 15–19 eV. Very different behavior in terms of lineshape and resonant enhancement is observed for the , and final states. This is explained by (1) the variation in the C–O bond lengths for the states involved in the electronic relaxation and (2) different contributions in terms of Mulliken population to the molecular orbitals determining the electronic character of the corresponding states. Since the final-state geometries are known from a number of previous experiments and ab initio calculations, the geometry of the C1s⁽⁻¹⁾π^*(1) intermediate states can be predicted in analogy with e.g. the N₂, CO₂ and N₂O molecules.     

Nonlinear bound-free pair creation in the strong electromagnetic fields of a heavy nucleus and an intense x-ray laser

We study e(-)e(+) pair creation in the collision of a heavy nucleus with an intense x-ray laser, where the produced e(-) is simultaneously captured into the K shell of the projectile nucleus. The parameters of the colliding system are chosen such that the absorption of at least two photons from the laser wave is required in order to surmount the energy threshold of the reaction. Considering this fundamental nonlinear strong-field process for the first time, we estimate the total production rate as well as the angular and energetic distributions of the emitted positrons. According to our results, the process of nonlinear bound-free pair creation could become observable by the aid of the upcoming x-ray laser facilities.     

强激光场中N2分子高次谐波的干涉效应

在强场近似下,利用Lewenstein模型研究了N2分子在强激光场中发射高次谐波的干涉效应,通过对N2分子产生的高次谐波和分子中单个原子产生高次谐波的比较,表明了干涉效应的存在. 得出随着高次谐波阶数的增加,干涉极小值会随着分子轴与激光偏振方向间夹角的增加而减小,在角度接近900附近时干涉效应消失,与两中心干涉模型预测的趋势一致. 通过分析高次谐波产生的机制和相位随取向角的变化,给出了干涉产生的原因.     

Role of rotational state-selected for nonadiabatic alignment: OCS molecules in femtosecond laser fields

Nonadiabatic alignment by intense nonresonant laser fields is a versatile technique to manipulate the spatial direction of molecules. By solving the time-dependent Schrödinger equation numerically the degree of alignment of the molecules initially in different rotational state are calculated and the results show that the degree of alignment strongly depends on the initial rotational state. Thus, the present study indicates that, for obtaining a high degree of alignment for molecules, appropriate selection of molecular rotational states is necessary.     

Resonant charging of Xe clusters in helium nanodroplets under intense laser fields

We theoretically investigate the impact of multiple plasmon resonances on the charging of Xe clusters embedded in He nanodroplets under intense pump-probe laser excitation (τ = 25 fs, I ₀ = 2.5 × 10¹⁴   W/cm², λ = 800 nm). Our molecular dynamics simulations on Xe₃₀₉He_10 000 and comparison to results for free Xe₃₀₉ give clear evidence for selective resonance heating in the He shell and the Xe cluster, but no corresponding double hump feature in the final Xe charge spectra is found. Though the presence of the He shell substantially increases the maximum charge states, the pump-probe dynamics of the Xe spectra from the embedded system is similar to that of the free species. In strong contrast to that, the predicted electron spectra do show well-separated and pronounced features from highly efficient plasmon assisted electron acceleration for both resonances in the embedded clusters. A detailed analysis of the underlying ionization and recombination dynamics is presented and explains the apparent disaccord between the resonance features in the ion and electron spectra.     

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.     

Kinetic energy release of diatomic and linear triatomic molecules in intense femtosecond laser fields

The kinetic energy release of fragment ions produced by the interaction of femtosecond laser pulse radiation with diatomic and linear triatomic molecules N_2, CO, CO_2 and CS_2 is investigated. In the case of linear polarization, angles at which the kinetic energy release of ions has the maximum value are different from the alignment of molecules though the kinetic energy release of fragment atomic ions depends on the angle between the laser polarization vector and the detection axis of the time-of-flight. For the diatomic molecules, the critical internuclear distance in multielectron dissociative ionization with a circularly polarized light is larger than that with a linearly polarized light. For linear triatomic molecules, our data indicate that a concerted Coulomb explosion process is a universal phenomenon in the interaction of molecules with intense laser fields, even in the circularly polarized regime. During two C－O (or C－S) bonds breaking simultaneously, the C ion obtained larger energy in circular polarization than that in the linear polarization. Different variations of kinetic energy release between the diatomic and the linear triatomic molecules are discussed.     

Enhanced ionization of vibrational hot carbon disulfide molecules in strong femtosecond laser fields

By using a heated molecular beam in combination with a time-of-flight mass spectrometer, we experimentally study the ionization of vibrational-hot carbon disulfide(CS_2) molecules irradiated by a linearly polarized 800-nm 50-fs strong laser field. The ion yields are measured in a laser intensity range of 7.0 × 10~(12) W/cm~2–1.5 × 10~(14) W/cm~2 at different molecular temperatures of up to 1400 K. Enhanced ionization yield is observed for vibrationally excited CS_2 molecules.The results show that the enhancement decreases as the laser intensity increases, and exhibits non-monotonical dependence on the molecular temperature. According to the calculated potential energy curves of the neutral and ionic electronic states of CS_2, as well as the theoretical models of molecular strong-field ionization available in the literature, we discuss the mechanism of the enhanced ionization of vibrational-hot molecules. It is indicated that the enhanced ionization could be attributed to both the reduced ionization potential with vibrational excitation and the Frank–Condon factors between the neutral and ionic electronic states. Our study paves the way to understanding the effect of nuclear motion on the strongfield ionization of molecules, which would give a further insight into theoretical and experimental investigations on the interaction of polyatomic molecules with strong laser fields.     

Dissociation of molecules in intense laser beam

Dissociation of molecules in the strong laser beam at the intensity of 10¹³–10¹⁴ W/cm² is investigated. Experimentally, the fragmentation of neutral molecules, CH₄, C₂H₄, C₄H₈; and the disintegration of molecular ions, CH ₄ ⁺ are studied by fluorescence spectroscopy and mass spectroscopy respectively. Some new phenomena, the strong dependence on the laser intensity, the universal dissociation, and the thorough fragmentation, are found in the fragmentation, and cannot be explained by the existing theories, as Coulomb Explosion theory or Re-scattering theory. We have suggested two new theories. The Super-excited State (SES) theory interprets the neutral fragmentation of molecules, which is stimulated to the SES by intense laser pulse. The Morse potential energy surface of the SES shows that either direct dissociation or pre-dissociation can take place in the SESs. Another theory, the theory of Field-assisted Dissociation (FAD) interprets the fragmentation of ionic molecules. According to this theory, the electric field of the laser pulse is involved directly to the dissociation process. QCT calculations for the trajectories moving on the dressed PES are performed. The result shows that the chemical bond which is parallel to the laser field vector undergo dissociation spontaneously. The dissociation takes place around 100 fs, which is in agreement with the ultrafast measurement in the pump-probe experiment.     

Photofragmentation of Na2+ in intense femtosecond laser fields: from photodissociation on light-induced potentials to field ionization.

Photofragmentation of Na2 + molecules in well prepared vibrational levels has been studied employing intense ( 10(11)-10(14) W/cm2) and ultrashort (80 fs) 790 nm laser fields. Four fragmentation channels with different released kinetic energies are observed. Depending on the applied laser intensity, the fragmentation of Na2 + is governed by photodissociation on light-induced potentials and field ionization followed by Coulomb explosion. Below 1x10(12) W/cm2, only photodissociation on light-induced potentials is seen. For intermediate laser intensities, field ionization at large internuclear distances competes with photodissociation, thus preventing the observation of above threshold dissociation. Field ionization at small internuclear distances dominates for the highest laser intensities used.     

Angular distributions of the fragments from coulomb explosions of diatomic molecules in intense laser fields

The angular distributions of the fragments from a Coulomb explosion of a diatomic heteronuclear molecule during multielectron dissociative ionization in a superintense field are considered in terms of classical mechanics. The patterns of angular distributions of the Coulomb explosion fragments are shown to differ in different ranges of laser pulse parameters. In particular, there are two distinct modes of fragment separation: separation in a Coulomb field and separation in the field of an effective “fragment + field” potential. The effective potential includes both the force of Coulomb repulsion between the fragments and the period-averaged force exerted on the system by the field; it can be determined by using the Kramers-Henneberger method. The limits of applicability of the Kramers-Henneberger method to the problem in question are discussed. These limits specify the range of field parameters in which the fragments fly apart in a direction perpendicular to the field for the initially arbitrary orientation of the molecular axis relative to the field.     

强激光场中真空极化效应

 通过求解狄拉克方程,对强激光场下真空极化问题进行了研究。理论计算结果表明：在仅随时间变化的电场下,要激发狄拉克海中负能级的电子,需要两个阈值条件,即激光场的电场强度大于等于10¹⁶ V/cm和激光场的持续时间大于等于10^-21 s。前者主要保证负能态电子有足够的能量跃迁到正能态,后者主要是保证电子在跃迁过程中动量亏损得以补偿。     

强激光场中真空极化效应

通过求解狄拉克方程,对强激光场下真空极化问题进行了研究。理论计算结果表明：在仅随时间变化的电场下,要激发狄拉克海中负能级的电子,需要两个阈值条件,即激光场的电场强度大于等于1016 V/cm和激光场的持续时间大于等于10-21 s。前者主要保证负能态电子有足够的能量跃迁到正能态,后者主要是保证电子在跃迁过程中动量亏损得以补偿。     

Nonsequential double recombination in intense laser fields

A second plateau in the harmonic spectra of laser-driven two-electron atoms is observed both in the numerical solution of a low-dimensional model helium atom and using an extended strong field approximation. It is shown that the harmonics well beyond the usual cutoff are due to the simultaneous recombination of the two electrons, which were emitted during different, previous half-cycles. The new cutoff is explained in terms of classical trajectories. Classical predictions and the time-frequency analysis of the ab initio quantum results are in excellent agreement. The mechanism corresponds to the inverse single photon double ionization process in the presence of a (low frequency) laser field.     

Xenon clusters in intense VUV laser fields

A simple model is developed that quantitatively describes intense interactions of a vacuum ultraviolet (VUV) laser pulse with a xenon cluster. We find good agreement with a recent experiment [Nature (London) 420, 482 (2002)]]. In particular, the large number of VUV photons absorbed per atom, at intensities significantly below 10(16) W/cm(2), is now understood.     

Rotation and alignment of diatomic molecules and their molecular ions in strong laser fields

A theory of classical rotation and alignment of diatomic molecules with and without permanent dipole moments and of their molecular ions in strong laser fields is developed. The actions of both cw and pulsed laser fields is considered. Conditions under which molecular axes are aligned with the field, which is presumed to be linearly polarized, have been determined. The analysis leads to a conclusion that molecules exposed to ultrashort laser pulses continue to rotate even after the end of the laser pulse. The effect of dynamical chaos on the rotational angular velocity in strong laser field is discussed. Zh. éksp. Teor. Fiz. 113, 573–582 (February 1998)