The dissociative ionization and Coulomb explosion of ethane by a femtosecond laser field

Femtosecond laser-induced dissociation and Coulomb explosion of polyatomic molecule C_2H_6 were systematically investigated using a time-of-flight mass spectrometer and a chirped pulse amplifier laser. With the laser intensity varying from 2.4×10^{15}W/cm^{2} to 1.2×10^{16}W/cm^2, strong molecular ions C_2H_n^+ (n=0－6) and atomic ions C^{m+} (m=1－3) signals were observed. The double-peak structure of atomic ions indicated the occurrence of Coulomb explosion. Compared with the nearly isotropic distribution of C^{+}, highly charged ions C^{m+} (m=2－3) exhibited a sharply anisotropic angular distribution, which was attributed to the geometric alignment.     

Field-induced ionization and Coulomb explosion of nitrogen

Femtosecond-laser field-induced ionization and Coulomb explosion of diatomic nitrogen were systematically investigated using time-of-flight mass and photoelectron spectrometry. Both linearly and circularly polarized femtosecond laser pulses were used at intensities varying from 5×10¹³ to 2×10¹⁵ W/cm². Strong N₂ ⁺, N₂ ²⁺, N⁺, N²⁺ and N³⁺ ion signals were observed for horizontally polarized pulses. Moreover, signals from the atomic ions exhibited a double-peak structure. Suppression of ionization was observed for circularly polarized pulses, while for vertically polarized pulses, only N₂ ⁺ and N₂ ²⁺ ions were observed. The angular distributions of the ions were measured under zero-field conditions in the ionization zone. The atomic ions N⁺, N²⁺ and N³⁺ exhibited highly anisotropic distributions, with maxima along the laser polarization vector and zeroes normal to the laser polarization vector. In contrast to the atomic ions, N₂ ⁺ exhibited a strong isotropic angular distribution. These observations indicate that dynamic alignment is responsible for the observed anisotropic angular distribution of the atomic ions. The kinetic energy spectrum of the photoelectrons is featureless and broad, extending above the ponderomotive potential of the laser pulse. The angular distribution is markedly anisotropic, with a maximum along the laser polarization vector. These observations further support the notion that the field-ionization mechanism is dominant under our experimental conditions. Received: 29 January 2002 / Revised version: 15 March 2002 / Published online: 12 July 2002     

Ultrafast Coulomb explosion imaging of molecules

Multiple ionization of small molecules leads to multifragmentation called Coulomb explosion. The atomic positions prior to the fragmentation event are determined from the multicharged fragments trajectories. Following the pioneering contribution of Prof. N.B. Delone on atomic ionization using strong laser fields, intense femtosecond laser pulses in the 10¹⁵ W cm^?2 range permit an efficient removal of valence electrons. Pulse durations have to be reduced to a few cycles in order to avoid any significant molecular stretching during multiple ionization. Pumpprobe excitation schemes offer promising perspectives for straightforward ultrafast Coulomb explosion imaging of excited and ionized molecular species.     

Dissociation and ionization of H+2 by ultrashort intense laser pulses probed by coincidence 3D momentum imaging

Laser-induced dissociation and ionization of H(+)(2) were simultaneously measured using coincidence 3D momentum imaging, allowing direct separation of the two processes, even where the fragment kinetic energy is the same for both processes. The results for 45 and 135 fs 790 nm pulses with an intensity of approximately 2.5 x 10(14) W/cm(2) differ from each other much more than one would expect from previous measurements with longer pulses. Ionization was negligible for the longer pulse and was strongly aligned along the laser polarization for the shorter pulse, but showed no structure in its kinetic energy distribution. In addition, the ionization to dissociation ratio was found to be much smaller than theoretically predicted for H(+)(2).     

Energetic-ion generation by the combination of laser pressure and Coulomb explosion

A scheme of generating energetic ions by the interaction of an ultrahigh-intensity laser pulse and a thin solid foil is studied. The combination of the effects of radiation pressure and Coulomb explosion makes the ion acceleration more effective. The maximum ion velocity variation with time is predicted theoretically while the temporal evolution of the electrostatic field due to the Coulomb explosion is taken into consideration. Two-dimensional particle-in-cell simulations are done to verify the theory.     

Coulomb explosion of CS_2 molecule under an intense femtosecond laser field

We experimentally demonstrate the Coulomb explosion process of CS_2 molecule under a near-infrared(800 nm)intense femtosecond laser field by a DC-sliced ion imaging technique. We obtain the DC-sliced images of these fragment ions S~+, S~(2+), CS~+, and CS~(2+)by breaking one C–S bond, and assign their Coulomb explosion channels by considering their kinetic energy release and angular distribution. We also numerically simulate the dissociation dynamics of parent ions CS_2~(k+)(k = 2–4) by a Coulomb potential approximation, and obtain the time evolution of Coulomb energy and kinetic energy release, which indicates that the dissociation time of parent ions CS_2~(k+) decreases with the increase of the charge number k.These experimental and theoretical results can serve as a useful benchmark for those researchers who work in the related area.     

Routes to control of H2 Coulomb explosion in few-cycle laser pulses

We have measured coincident ion pairs produced in the Coulomb explosion of H2 by 8-30 fs laser pulses at different laser intensities. We show how the Coulomb explosion of H2 can be experimentally controlled by tuning the appropriate pulse duration and laser intensity. For laser pulses less than 15 fs, we found that the rescattering-induced Coulomb explosion is dominated by first-return recollisions, while for longer pulses and at the proper laser intensity, the third return can be made to be the major one. Additionally, by choosing suitable pulse duration and laser intensity, we show H2 Coulomb explosion proceeding through three distinct processes that are simultaneously observable, each exhibiting different characteristics and revealing distinctive time information about the H2 evolution in the laser pulse.     

Ultrafast Coulomb explosion imaging of molecules and molecular clusters

Taking an image of their structure and a movie of their dynamics of small quantum systems have always been a dream of physicists and chemists. Laser-induced Coulomb explosion imaging (CEI) provides a great opportunity to make this dream a reality for small molecules or their aggregation —— clusters. The method is unique for identifying the atomic locations with ångstrom spatial resolution and capturing the structural evolution with a femtosecond time scale, in particular for imaging transient state products. This review summarizes the determination of three-dimensional equilibrium geometry of molecules and molecular cluster system through the reconstruction from the fragments momenta, and also shows that the dissociation dynamics on the complex potential energy surface can be tracked in real-time with the ultrafast CEI (UCEI). Furthermore, the detailed measurement and analysis procedures of the CEI, theoretical methods, exemplary results, and future perspectives of the technique are described.     

Theoretical investigation of 2+2 resonance enhanced multi-photon ionization probability

The analytic formula of the ionization probability in the process of 2+2 resonance enhanced multi-photon ionization (REMPI) is derived from the dynamic rate equation about the interaction of photon and material. Based on the formula, the influence of laser intensity, laser pulse duration and collision relaxation rate on the ionization probability is investigated theoretically. It is shown that the ionization probability increases with the laser intensity and laser pulse duration. The ionization probability will get to one until two steps saturation with the increase of laser intensity. After that, the ionization probability will oscillates narrowly around the saturation value if the laser intensity increases further. The results also show that the ionization probability will decrease in linear manner nearly with the increase of collision relaxation rate. But the variation is small. So the influence of the collision relaxation rate (or even sample pressure) on the ionization probability can be ignored. In the practical use of REMPI, higher sample pressure will reduce the intensity of the detection signal is due to the collision complex of the positive and negative ions. This will reduce the collection efficiency of the ions, and influence the magnitude of the ion signal further.     

基于共振增强多光子电离技术的慢电子速度影像应用

利用激光共振增强多光子电离技术,我们既可以观察中性物种激发态的振动结构也可以获得相应正离子的高分辨电子能谱.采用自行研制的双静电透镜系统对Xe原子在258.00 nm激光束下的三光子电离过程展开研究,优化得到飞行时间质谱的质量分辨率(m/Δm)达到1300,慢电子速度成像的电子能量分辨率(ΔE/E)为2.4%,阈值电子能量分辨优于1 me V.在该条件下,开展了分子的电子谱研究,研究了苯的激发电子态共振增强双光子电离光谱和振动态选择的苯正离子的慢电子速度成像谱,通过对谱线归属,获得了1B2u激发态的振动序列和苯正离子的振动能级结构信息.     

基于共振增强多光子电离技术的慢电子速度影像应用

利用激光共振增强多光子电离技术,我们既可以观察中性物种激发态的振动结构也可以获得相应正离子的高分辨电子能谱。采用自行研制的双静电透镜系统对Xe原子在258.00nm激光束下的三光子电离过程展开研究,优化得到飞行时间质谱的质量分辨率(m/Δm)达到1300,慢电子速度成像的电子能量分辨率（ΔE/E）为2.4%,阈值电子能量分辨优于1 meV。在该条件下,开展了分子的电子谱研究,研究了苯的激发电子态共振增强双光子电离光谱和振动态选择的苯正离子的慢电子速度成像谱,通过对谱线归属,获得了1B2u激发态的振动序列和苯正离子的振动能级结构信息。     

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.     

稀土元素铕(Fu)的单光子共振和双光子共振激光增强电离光谱

本文首次报道稀土元素铕(Eu)的激光增强电离光谱.用紫外可调谐激光器检测到EuI 287.779um,EnI 287·887nm,EuI 289.254nm,Eul 289.303nm,EuI 289.383nm的单光子共振激光增强光谱.用可见区可调谐染料激光器检测到EuI的双光子共振激光增强电离光谱.对铕(Eu)原子激发和离化机理进行了讨论.稀土元素铕的检测限达10ng/ml.     

Collisionless multiphoton ionization of water molecules by a TEACO2 laser

Collisionless ionization of water molecules into fragments of H⁺, H₂⁺, O⁺, OH⁺, H₂O⁺ were observed using a high power TEACO₂ laser. The mechanism could be related to that of selective dissociation of complex molecules by the same laser.     

Femtosecond laser-induced dynamic alignment in Coulomb explosion of CO: Roles of laser wavelength, intensity and pulse duration

Dependences of dynamic alignment of CO molecules induced by intense femtosecond laser fields on laser wavelength, intensity and pulse duration are investigated by numerical simulations. A counting approach and a fourth-order Runge-Kutta algorithm are used to calculate the angular distribution and the time evolution of molecules. A two-step Coulomb explosion model of diatomic molecules in intense laser fields is used to determine the instant that CO molecular dynamic alignment is over. Our calculating results show that the linear polarizability and the damping force play an important role in the angular rotation of CO molecule in conditions of 800 nm laser wavelength and 10¹⁵ W/cm² laser intensity. The contributions of the second-order field-induced dipole moment and the higher-order correction term to molecular rotation acceleration comparing to the linear polarizability and damping force are negligible. The extent of dynamic alignment of CO molecules reduces with the increasing of laser intensity. The dynamic alignment time of CO molecules is tightly connected to the laser pulse duration. The angular distributions of CO molecules as the laser pulse length varied from 50 to 250 fs at laser intensity of 3×10¹⁴ W/cm² are shown and discussed.     

Tabletop nucleosynthesis driven by cluster Coulomb explosion

Coulomb explosion of completely ionized (CH4)n, (NH3)n, and (H2O)n clusters will drive tabletop nuclear reactions of protons with 12C6+, 14N7+, and 16O8+ nuclei, extending the realm of nuclear reactions driven by ultraintense laser-heterocluster interaction. The realization for nucleosynthesis in exploding cluster beams requires complete electron stripping from the clusters (at laser intensities I(M) > or = 10(19) W cm(-2)), the utilization of nanodroplets of radius 300-700 A for vertical ionization, and the attainment of the highest energies for the nuclei (i.e., approximately 30 MeV for heavy nuclei and approximately 3 MeV for protons).     

Selective ultratrace analysis of 41Ca by laser resonance ionization

A compact resonance ionization mass spectrometer is presented. It is presently applied for sensitive and highly selective ultratrace determination of the long-lived radioisotope ⁴¹Ca for environmental, biological, and fundamental investigations. The development of coherent multistep resonance ionization enables the realization of experimental detection limits as low as10⁶ atoms per sample and very high isotopic selectivity above 10¹². This revised version was published online in August 2006 with corrections to the Cover Date.     

Coulomb exploded directional double ionization of N_2O molecules in multicycle femtosecond laser pulses

We experimentally investigate Coulomb exploded directional double ionization of N_2O molecules in elliptically polarized femtosecond laser pulses.The denitrogenation and deoxygenation channels are accessed via various pathways.It leads to distinct asymmetries in directional breaking of the doubly ionized N_2O molecules versus the instantaneous laser field vector, which is revealed by tracing the sum-momentum spectra of the ionic fragments as a recoil of the ejected electrons.Our results demonstrate that the accessibility of the Coulomb exploded double ionization channels of N_2O molecules are ruled by the detailed potential energy curves, and the directional emission of the fragments are governed by the joint effects of the electron localization-assisted enhanced ionization of the stretched molecules and the profiles of the molecular orbitals.     

Dynamics of Coulomb explosion of hydrogen clusters in a high-intensity femtosecond laser pulse

Using Bethe model, the dynamics of the ionization and Coulomb explosion of hydrogen clusters (0.5-5nm) in high-intensity (1015-1017 W/cm2) femtosecond laser pulses have been studied theoretically, and the dependence of energy of protons emitted from exploding clusters on cluster size and laser intensity has been investigated. It is found that the maximum proton energy increases exponentially with the cluster size, and the exponent is mainly determined by the laser intensity. For a given cluster size, the maximum proton energy increases with increasing laser intensity and gets saturation gradually. The calculation results are in agreement with the recent experimental observation.     

Ultra-short laser ablation of metals and semiconductors: evidence of ultra-fast Coulomb explosion

We have studied ultra-fast laser ablation of Si and a metal via the neutral and ion yield, the energy distribution of emitted neutrals and the charge distribution as a function of the laser pulse width. Two processes, one leading to the ejection of fast (3–7 eV), the other to slow thermal particles, can be identified. The origin of the first process can be correlated with laser pulse widths (or pump–probe delays) and processes on a time scale below 100 fs. Results for Si confirm recent findings for Coulomb explosion (CE) and we show for the first time that CE exists as a mechanism of material removal from metals for ultra-short laser pulses. PACS 06.60.Jn; 79.20.Ds; 79.60.Bm; 42.62.Fi; 71.20.-b