飞秒强激光场中分子双电离的半经典动力学模拟

文章介绍了超短强激光场中原子、分子双电离的研究现状,提出了能够有效处理双电离过程的半经典模型,成功地重现了双电离率随激光强度变化的实验数据,同时预言了分子取向对双电离率的重要影响.文章还通过分析典型的双电离轨道的演化,给出了理解双电离复杂动力学过程的直观物理图像.     

Recollision dynamics and phase diagram for nonsequential double ionization with circularly polarized laser fields

A semiclassical quasistatic model is used to investigate the recollision dynamics in circularly polarized laser fields. A velocity window for recollision to occur is found. Only when the return electron's orbits are irregular does significant double ionization take place. The model reproduces the experimental results for magnesium and explains the apparently conflicting experimental results in terms of an analytical formula that demarcates the phase diagram for the nonsequential double ionization in circularly polarized laser fields.     

Simulation of laser ablation in aluminum: the effectivity of double pulses

Lasers are becoming a more and more important tool in cutting and shaping materials. Improving precision and effectivity is an ongoing demand in science and industry. One possibility is double pulses. Here, we study laser ablation of aluminum by the two-temperature model. There the laser is modeled as a source in a continuum heat conduction equation for the electrons, whose temperature then is transferred to a molecular dynamics particle model by an electron–phonon coupling term. The melting and ablation effectivity is investigated depending on the relative intensity and the time delay between two Gaussian shaped laser pulses. It turns out that at least for aluminum the optimal pulse shapes are standard Gaussian pulses. For double pulses with delay times up to 200 ps, we find a behavior as observed in experiment: The ablation depth decreases beyond a delay of 10 ps even if one does not account for the weakening at the second pulse due to laser–plasma interaction.     

Titanium plasma spectroscopy studies under double pulse laser excitation

Laser-induced breakdown spectroscopy (LIBS) was applied for parametric studies of titanium (Ti) plasma using single and double pulsed laser excitation scheme. Here a pulsed Nd:YAG laser was employed for generation of laser produced plasma from solid Ti target at ambient pressure. Several ionized titanium lines were recorded in the 312–334 nm UV region. The temporal evolution of plasma parameters such as excitation temperature and electron number density was evaluated. The effect of incident laser irradiance, position of the laser beam focal point with respect to the surface of illumination, single and double laser pulse effect on plasma parameters were also investigated. This study contributes to a better understanding of the LIBS plasma dynamics of the double laser pulse effect on the temporal evolution of various Ti emission lines, the detection sensitivity and the optimal dynamics of plasma for ionized states of Ti. The results demonstrate a faster decay of the continuum and spectral lines and a shorter plasma life time for the double pulse excitation scheme as compared with single laser pulse excitation. For double pulse excitation technique, the emissions of Ti lines intensities are enhanced by a factor of five which could help in the improvement of analytical performance of LIBS technique. In addition, this study proved that to avoid inhomogeneous effects in the laser produced plasma under high laser intensities, short delay times between the incident laser pulse and ICCD gate are required.     

Bifurcation of ion momentum distributions in sequential double ionization by elliptically polarized laser pulses

Using a fully classical model, we have studied sequential double ionization (SDI) of argon driven by elliptically polarized laser pulses at intensities well in the over-barrier ionization region. The results show that the width of the ion momentum along the major elliptical axis increases with the ellipticity while that in the laser propagation direction decreases with the ellipticity. The ion momentum in the minor elliptical axis bifurcates from one peak structure to three-peak, then to four-peak, finally to six-peak structure. Analysis shows that this ellipticity dependence of the ion momentum distribution is a result of the subcycle nature of the ionization dynamics in SDI. By changing the ellipticity and wavelength of the driving pulses, this subcycle ionization dynamics is more observable. This provides a simple and efficient way to study the subcycle ionization dynamics in strong field processes.     

Multiple recollisions in nonsequential double ionization below the recollision-ionization threshold

By using the three-dimensional classical ensemble model, the recollision dynamics in nonsequential double ionization (NSDI) of Ar by 780-nm laser pulses at (6-1.2)×10¹⁴ W/cm² was extensively studied. We revealed the picture of multiple-recollision in the double ionization events at the laser intensity region below the recollision-ionization threshold. Via tracing the NSDI trajectories, it was found that the contribution of these multiple-recollision events increases as the laser intensity decreases. In this low intensity region, many multiple-recollision induced NSDI trajectories occur through the doubly excited states. The decay speed of the doubly excited state decreases with the decreasing laser intensity.     

Generation of XUV attosecond pulses in the process of atomic ionization by few-cycle laser radiation

Ionization of a model two-electron atom in the presence of a strong field of ultrashort laser pulses is investigated using the numerical integration of the nonstationary Schrödinger equation, which describes the dynamics of a quantum system in the presence of an electromagnetic wave. The features of two-electron ionization in the presence of one-and two-cycle pulses are analyzed. The suppression of double ionization in the presence of ultrashort laser pulses related to a finite-time interelectron energy exchange upon the laser action is demonstrated. The features of the generation of high-order harmonics and single XUV attosecond pulses are studied for the atomic ionization by few-cycle laser pulses. The parameters of the laser pulse are optimized for the effective generation of a single XUV attosecond pulse.     

Nonsequential double ionization of Xe by mid-infrared laser pulses

With the three-dimensional semiclassical ensemble model, we studied the correlated electron dynamics in strong-field nonsequential double ionization of Xe by mid-infrared laser pulses over a wide range of laser intensities. Numerical results show that the correlated electron momentum distribution exhibits the strong back-to-back pattern at the lower laser intensity. It evolves into the side-by-side behavior as the laser intensity increases and presents the experimentally observed crosslike shape at high laser intensity. Different from the case of near-infrared region where recollision mainly occurs at the first returning, at the mid-infrared region recollision dominantly occurs at the later returnings. The windows of initial transverse velocity for the various multiple-returning recollision trajectories are different and are unambiguously determined by this semiclassical ensemble model.     

Double Ionization Dynamics of Molecular Hydrogen in Ultrashort Intense Laser Fields

We experimentally investigate the double ionization of molecular hydrogen subjected to ultrashort intense laser pulses.The total kinetic energy release of the two coincident H~+ ions,which provides a diagnosis of different processes to double ionization of H_2,is measured for two different pulse durations,i.e.,25 and 5fs,and various laser intensities.It is found that,for the long pulse duration(i.e.,25 fs),the double ionization occurs mainly via two processes,i.e.,the charge resonance enhanced ionization and recollision-induced double ionization.Moreover,the contributions from these two processes can be significantly modulated by changing the laser intensity.In contrast,for a few-cycle pulse of 5fs,only the recollsion-induced double ionization survives,and in particular,this process could be solely induced by the first-return recollision at appropriate laser intensities,providing an efficient way to probe the sub-laser-cycle molecular dynamics.     

Laser-cluster-interaction in a nanoplasma-model with inclusion of lowered ionization energies

The interaction of intense laser fields with silver and argon clusters is investigated theoretically using a modified nanoplasma model. Single pulse and double pulse excitations are considered. The influence of the dense cluster environment on the inner ionization processes is studied including the lowering of the ionization energies. There are considerable changes in the dynamics of the laser-cluster interaction. Especially, for silver clusters, the lowering of the ionization energies leads to increased yields of highly charged ions.     

Peculiarities of the ionization of many-electron systems and generation of attosecond pulses in ultrashort laser fields

The ionization of a model two-electron atom in the field of a strong ultrashort laser pulse is studied by numerical integration of the nonstationary Schrödinger equation describing the dynamics of a quantum system in the field of an electromagnetic wave. Pecularities of the two-electron ionization are analyzed for pulses whose duration amounts to one to two periods of oscillation of the electric field of the wave at different frequencies of the incident radiation. For extremely short pulses, the double ionization is found to be suppressed. This effect is caused by the finiteness of the interelectron energy exchange time during the laser action. Peculiarities of the generation of high-order harmonics and single XUV attosecond pulses upon ionization of atoms by laser pulses, whose duration is within one to two optical cycles, are investigated.     

Control of Ionization in the Interaction of Strong Laser Fields with Dense Nanoplasmas

Different experimental methods to maximize the yield of highly charged ions in silver and xenon clusters interacting with intense and ultra‐short optical laser pulses are discussed. Theoretically, the interaction of strong laser fields with clusters is investigated within the nanoplasma model. The time evolution of the laser intensity has been parametrized. The free optimization of the parameters with a genetic algorithm is an effective but expensive tool to control the plasma dynamics. Comparison is given to the parametric control method in which pulse separation and relative intensity ratio of double‐pulses are varied. This method delivers in the case of silver and xenon clusters pulses quite close to the optimal pulse shape (© 2011 WILEY‐VCH Verlag GmbH & Co. KGaA, Weinheim)     

Microscopic Dynamics of Nonsequential Double Ionization by Elliptically Polarized Few-Cycle Laser Pulses

With the classical ensemble model, we investigate nonsequential double ionization (NSDI) of xenon atoms using 780 nm, 0.25 PW/cm2elliptically polarized few-cycle laser pulses. The momentum distribution of correlated electron along the long axis of the laser polarization plane shows an obvious V-like structure locating at the third quadrant, and the momentum along the short axis of the laser polarization plane are mainly distributed in the second and fourth quadrants. Moreover, we demonstrate that the Coulomb repulsion interaction plays a decisive role to the above results.By back analyzing the classical trajectories of NSDI, we find that there are two kinds of recollision trajectories mainly contribute to NSDI, and the different microscopic dynamics for the two kinds of trajectories are clearly explored.     

Observation of a transition in the dynamics of strong-field double ionization

The double ionization of argon and xenon in an intense laser field has been studied in detail using an electron-ion coincidence technique. The observed double ionization electron spectra in xenon show resonancelike structures here resolved for the first time. In argon, the featureless spectra are consistent with rescattering. This represents a clear transition in the dynamics of strong-field double ionization, analogous to the well-known transition between the tunneling and multiphoton regimes in single ionization.     

Ab initio calculation of the double ionization of helium in a few-cycle laser pulse beyond the one-dimensional approximation

We present ab initio computations of the ionization of two-electron atoms by short pulses of intense linearly polarized Ti:sapphire laser radiation beyond the one-dimensional approximation. In the model the electron correlation is included in its full dimensionality, while the center-of-mass motion is restricted along the polarization axis. Our results exhibit a rich double ionization quantum dynamics in the direction transversal to the field polarization, which is neglected in the previous models based on the one-dimensional approximation.     

Controlling attosecond double ionization dynamics via molecular alignment

We investigate the dynamics of double ionization in aligned nitrogen molecules. An ultrashort, weak laser pulse creates an aligned ensemble of molecules that is ionized with a subsequent, strong probe pulse. We find that the two electrons involved in nonsequential double ionization more likely exit the molecule in the same direction if it is parallel to the probe laser polarization, indicating that they are ejected within a few hundred attoseconds of each other. Double ionization is less probable and takes longer for perpendicular molecules.     

Minimization of cavitation effects in pulsed laser ablation illustrated on laser angioplasty

Cavitation effects in pulsed laser ablation can cause severe deformation of tissue near the ablation site. In angioplasty, they result in a harmful dilatation and invagination of the vessel walls. We suggest to reduce cavitation effects by dividing the laser pulse energy into a pre-pulse with low and an ablation pulse with high energy. The pre-pulse creates a small cavitation bubble which can be filled by the ablation products of the main pulse. For suitable energy ratios between the pulses, this bubble will not be enlarged by the ablation products, and the maximal bubble size remains much smaller than after a single ablation pulse. The concept was analyzed by numerical calculations based on the Gilmore model of cavitation dynamics and by high-speed photography of the effects of single and double pulses performed with a silicone tube as vessel model. The use of double pulses prevents the deformation of the vessel walls. The concept works with an energy ratio of up to about 1:30 between the pulses. For the calculated optimal ratio of 1:14.6, the bubble volume is reduced by a factor of 17.7. The ablation pulse is best applied when the pre-pulse bubble is maximally expanded, but the timing is not very critical.     

Binary and recoil collisions in strong field double ionization of helium

We have investigated the correlated momentum distribution of both electrons from nonsequential double ionization of helium in a 800 nm, 4.5 x 10(14 W/cm2 laser field. Using very high resolution coincidence techniques, we find a so-far unobserved fingerlike structure in the correlated electron momentum distribution. The structure can be interpreted as a signature of the microscopic dynamics in the recollision process. We identify features corresponding to the binary and recoil lobe in field-free (e,2e) collisions. This interpretation is supported by analyzing ab initio solutions of a fully correlated three-dimensional helium model.     

Double pulse UV laser induced breakdown spectroscopy of stainless steel

Results of experimental investigations of 304 austenitic stainless steel (ASS) ultraviolet spectral range by single and double pulse laser induced breakdown spectroscopy (LIBS) at atmospheric pressure are reported. Various parameters, such as laser energy, placement of the laser beam focus with respect to the surface of illumi-nation, and collinear double laser pulse delay were used as variables. This study contributes to a better under-standing of the LIBS plasma dynamics by observing the temporal evolution of various emission lines. Temperature measurements were made by the Boltzmann diagram method using singly ionized Fe lines, and electron densities were found from Stark broadening. The temporal behaviors of these parameters were also estimated. It was found that the electron temperature for double pulses is higher than that for single pulse of the same total energy. For double pulse LIBS, the iron line emission intensities are enhanced and the analytical performance is improved. For instance, the intensity of iron line Fe I 275.01 nm was a factor of about 300 times higher if a double pulse of 2 × 20 mJ was used instead of a single pulse of 40 mJ when focusing the beam 4.7 mm behind the target surface. Published in Zhurnal Prikladnoi Spektroskopii, Vol. 79, No. 5, pp. 654–660, 2006.