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).     

纳秒强激光电离苯产生高价碳离子的波长效应

随着高强度超短脉冲激光器的发展 ,分子、原子与强激光场的相互作用已经成为一个重要的研究领域 ,其中分子或原子团簇在强场下发生的库仑爆炸现象成为研究的热点之一 .苯具有高对称的环形结构 ,激发态能级密集 ,因此 ,不论是早期的激光对分子的多光子电离解离 (MPID) ,以及强场与多原子分子的相互作用 ,还是后来超短脉冲激光下团簇相关的库仑爆炸研究都将其作为一个重要的研究对象[1- 8] .最近 ,我们用波长为 5 3 2nm、脉宽为 2 5ns的激光对苯等物质进行电离时 ,发现在 1 0 10 ～1 0 11W/cm2 的功率密度下 ,其质谱中出现了高平动能的C2 +…     

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.     

Electronic and nuclear responses of fixed-in-space H2S to ultrashort intense laser fields

The Coulomb explosion dynamics of H2S, H2S3+-->H+ +S+ + H+, in ultrashort intense laser fields (12 fs, approximately 2 x 10(14) W/cm2) is studied by the coincidence momentum imaging of the three fragment ions. Different electronic and nuclear responses are identified depending on the direction of laser polarization epsilon in the molecular frame. The dependence can be interpreted in terms of the electronic and bonding characters of charge transfer states of H2S coupled to the electronic ground state.     

Intense-laser-field ionization of the hydrogen molecular ions H2+ and D2+ at critical internuclear distances

Fragmentation of H2+ and D2+ in ion beams has been studied with short intense laser pulses (100 fs, I=5x10(13)-1x10(15) W/cm2) and by a high-resolution two-dimensional velocity imaging technique. In the Coulomb explosion channel, at intensities just above the threshold for this process, we observe a clear structure in the kinetic energy spectra not previously found or predicted. The peaks can be attributed to single vibrational levels. We interpret this observation as a dissociative allocation of the electron to a proton followed by enhanced ionization at a well-defined "critical" overstretched internuclear distance. When using longer pulses we observe three separate Coulomb explosion velocity groups corresponding to critical distances of about 8, 11, and 15 a.u.     

Attosecond strobing of two-surface population dynamics in dissociating H2+

Using H2+ and D2+, we observe two-surface population dynamics by measuring the kinetic energy of the correlated ions that are created when H2+ (D2+) ionize in short (40-140 fs) and intense (10(14) W/cm2) infrared laser pulses. Experimentally, we find a modulation of the kinetic energy spectrum of the correlated fragments. The spectral progression arises from a hitherto unexpected spatial modulation on the excited state population, revealed by Coulomb explosion. By solving the two-level time-dependent Schr?dinger equation, we show that an interference between the net-two-photon and the one-photon transition creates localized electrons which subsequently ionize.     

Jahn-Teller effect in the methane cation: Rovibronic structure and the geometric phase

The rovibronic structure in the photoelectron spectrum of CH4 has been assigned in infrared-vacuum ultraviolet double-resonance experiments and analyzed using an effective tunneling-rotation Hamiltonian. Comparison of theoretical and experimental level structures of CH4+ reveals the effect of the geometric phase and establishes that at low energies, the structure and dynamics are governed by a large-amplitude tunneling motion connecting equivalent minima of C(2v) geometry. The rotationless ground state of CH4+ is a tunneling doublet of triply degenerate levels and the lowest level has rovibronic symmetry F2. The adiabatic ionization energy of CH4 is 101753.0(15) cm(-1).     

Energetic heavy-Ion and proton generation from ultraintense laser-plasma interactions with solids

Heavy ions with energies up to 430+/-40 MeV have been measured from laser-solid interactions at focused intensities of up to 5x10(19) W/cm(2). Observations of proton emission indicate significant structure in the energy spectrum as well as an angular emission profile which varies with energy. Two qualitatively different components of ion emission are observed: (i) a high-energy component which is likely generated by a combination of "Coulomb explosion" and acceleration by the space charge force from hot electrons which escape the plasma, and (ii) a lower-energy component which forms a ring likely created by magnetic fields in the ablated plasma.     

Interaction of argon clusters with intense VUV-laser radiation: the role of electronic structure in the energy-deposition process

The response of Ar clusters to intense vacuum-ultraviolet pulses is investigated with photoion spec-troscopy. By varying the laser wavelength, the initial excitation was either tuned to absorption bands of surface or bulk atoms of clusters. Multiple ionization is observed, which leads to Coulomb explosion. The efficiency of resonant 2-photon ionization for initial bulk and surface excitation is compared with that of the nonresonant process at different laser intensities. The specific electronic structure of clusters plays almost no role in the explosion dynamics at a peak intensity larger than 1.8 x 10(12) W/cm(2). The inner ionization of atoms for resonant and nonresonant excitation is then saturated and the energy deposition is mainly controlled by the plasma heating rate. Molecular dynamics simulations indicate that standard collisional heating cannot fully account for the strong energy absorption.     

甲烷电离特性的等离子体发射光谱法研究

应用等离子体发射光谱法,用CCD(charge coupled device)光栅光谱仪记录并标识了脉冲电晕甲烷等离子体370～1 100 nm的发射光谱,确定了常温常压下高纯甲烷(99.99%)经100 kV, 100 Hz脉冲高压电离后的产物为H,C+,CH,C,C₂,C₃, C₄,C₅和烃等。通过分析实验检测到的甲烷等离子体发射光谱,给出了甲烷经脉冲高压电离形成电晕等离子体的机理和自由基CH_n(n=3,2,1)、碳、烃等产物的电离途径。结果显示甲烷分子经高能电子非弹性碰撞后脱氢程度很高,大量氢原子及其离子和甲烷自由基在进一步被高能电子作用下合成了烯烃、炔烃、烷烃和高聚碳化物。实验所获得的脉冲甲烷等离子体发射光谱及其机理分析可为甲烷及其转化研究提供相关依据。     

Time-resolved imaging and manipulation of H2 fragmentation in intense laser fields

We report on the experimental realization of time-resolved coincident Coulomb explosion imaging of H2 fragmentation in 10(14) W/cm(2) laser fields. Combining a high-resolution "reaction microscope" and a fs pump-probe setup, we map the motion of wave packets dissociating via one- or two-photon channels, respectively, and observe a new region of enhanced ionization. The long-term interferometric stability of our system allows us to extend pump-probe experiments into the region of overlapping pulses, which offers new possibilities for the manipulation of ultrafast molecular fragmentation dynamics.     

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.     

High energy proton ejection from hydrocarbon molecules driven by highly efficient field ionization

We investigated the ejection of energetic protons from a series of polyatomic hydrocarbon molecules exposed to 790 nm 27 fs laser pulses. Using multiparticle coincidence imaging we were able to decompose the observed proton energy spectra into the contributions of individual fragmentation channels. It is shown that the molecules can completely fragment already at relatively low peak intensities of a few 10(14) W/cm(2), and that the protons are ejected in a concerted Coulomb explosion from unexpectedly high charge states. The observations are in agreement with enhanced ionization taking place at many C-H bonds in parallel.     

Visualizing recurrently migrating hydrogen in acetylene dication by intense ultrashort laser pulses

We demonstrate the visualization of ultrafast hydrogen migration in deuterated acetylene dication (C2D2{2+}) by employing the pump-probe Coulomb explosion imaging with sub-10-fs intense laser pulses (9 fs, 0.13 PW/cm{2}, 800 nm). It is shown, from the temporal evolution of the momenta of the fragment ions produced by the three-body explosion, C2D2{3+}-->D{+} + C{+} + CD{+}, that the migration proceeds in a recurrent manner: the deuterium atom first shifts from one carbon site to the other in a short time scale (approximately 90 fs) and then migrates back to the original carbon site by 280 fs, in competition with the molecular dissociation.     

Low field laser ionization of argon clusters: the remarkable fragmentation dynamics of doubly ionized clusters

We have investigated the fission following a Coulomb explosion in argon clusters (up to Ar800) irradiated by a femtosecond infrared laser with moderate intensity IL approximately 10(13) W cm(-2). We report the a priori surprising observation of well-defined velocity distributions of the ionized fragments Ar+n<50. This is interpreted by the formation of a valence shell excited charged ion, followed by relaxation, charge transfer by autoionizing collision at very short distance, and asymmetric fission.     

532 nm激光作用下CH3I分子的多光子电离

利用飞行时间质谱仪在超声射流冷却条件下探讨了532 nm激光作用下CH3I分子的多光子电离(MPI)解离过程和机制,得到了分子的飞行时间质谱,质谱中包含较强的I 、CH3 离子信号和较弱的CH3I 、CHn (n≤2)、C 、H 离子信号.不同激光能量下的质谱信号在排布上相似,但在强度上有差别.在532 nm激光作用下CH3I分子的多光子电离包括两个过程:一是CH3I分子由双光子激发到A带解离,生成I原子和CH3基团,然后再吸收光子实现中性碎片电离;另一通道是CH3I分子由三光子共振激发到里德堡C态,处于激发态的母体分子继续吸收两个光子电离形成母体离子,碎片离子可由母体离子解离形成.     

Coulomb explosion of large polyatomic molecules assisted by nonadiabatic charge localization

The electron-nuclear dynamics of the Coulomb explosion of a large polyatomic molecule, anthracene, is probed using kinetic energy distributions of produced H+ ions. The kinetic energy release of ejected protons exceeds 30 eV for anthracene exposed to 10(14) W cm(-2), 800 nm pulses of 60 fs duration. We propose a strong-field charge localization model, based on nonadiabatic dynamics of charge distribution in a (multiply) ionized molecule; the charge localization lasts many laser periods and is sustained through successive ionizations of the molecular ion. The model explains quantitatively the dependence of the H+ kinetic energy on the laser intensity. Dissociative ionization of a polyatomic molecule enabled by long-lived charge localization is a new type of electron-nuclear dynamics and is essential for understanding the pathways of molecular or ionic fragmentation in strong fields.     

Response of polyatomic molecules to ultrastrong laser- and ion-induced fields

The exposure of molecules to short, ultrastrong electric fields leads to multiple ionization and a subsequent Coulomb explosion. We present a comparative study where uracil molecules are exposed to fields generated by high-power laser pulses (tau approximately 75 fs, I > 10(16) W/cm2) or swift highly charged ions (0.5 MeV Xe25+) representing a half-cycle pulse of less than 10 fs duration. Molecular dynamics and structural information contained in the fragmentation pathways can be assessed separately. Despite the similar field strengths large differences in fragment kinetic energies are found which are related to field shape and duration with the aid of molecular dynamics simulations.     

Ultrafast nuclear dynamics and non-uniform Coulomb explosion of heteroclusters

This paper reports on some unique features of the ion spatial distribution, energetics and time-resolved dynamics in Coulomb explosion of multicharged light-heavy heteroclusters, consisting of light, low-charge and heavy, high-charge, ions, e.g. hydroiodic acid [image omitted] and its isotopic substituents [image omitted] and [image omitted]. In these clusters, extreme multielectron ionization in ultraintense laser fields (peak intensity I = 1015 - 1020 W cm-2) results in highly charged heavy ions, e.g. qI ? 7 at I = 6×1015 W cm-2 and qI = 25 at I = 1019 W cm-2. Molecular dynamics simulations based on the cluster vertical ionization (CVI) initial conditions, together with complete simulations involving both electron and nuclear dynamics of heteroclusters subjected to a Gaussian laser pulse, which were conducted for Coulomb explosion of [image omitted] and [image omitted] ionic clusters, reveal expanding, thin, two-dimensional spherical shells of the light D+ or H+ ions, with the monolayer expansion occurring on the femtosecond time scale. The expanding spherical nanoshells of light ions are analogous to a 'soap bubble', characterized by negative surface tension and driven by Coulomb pressure. The energetic data for the light ions reveal high energies with a narrow energy distribution, characterized by a lower energy cut-off, e.g. average energy Eav = 23 keV at width ΔE/Eav = 0.16, and a cut-off energy of EMIN = 19.2 keV for Coulomb explosion of [image omitted] clusters. These dynamic, structural and energetic data for exploding multicharged light-heavy heteroclusters arise from kinematic overrun effects of the light ions.