Kimika Fakultatea, Euskal Herriko Unibertsitatea and Donostia International Physics Center (DIPC), Donostia, Euskadi, Spain.
J Chem Phys. 2011 Feb 21;134(7):074315. doi: 10.1063/1.3521476.
We report on the calculations of kinetic energy distribution (KED) functions of multiply charged, high-energy ions in Coulomb explosion (CE) of an assembly of elemental Xe(n) clusters (average size (n) = 200-2171) driven by ultra-intense, near-infrared, Gaussian laser fields (peak intensities 10(15) - 4 × 10(16) W cm(-2), pulse lengths 65-230 fs). In this cluster size and pulse parameter domain, outer ionization is incomplete∕vertical, incomplete∕nonvertical, or complete∕nonvertical, with CE occurring in the presence of nanoplasma electrons. The KEDs were obtained from double averaging of single-trajectory molecular dynamics simulation ion kinetic energies. The KEDs were doubly averaged over a log-normal cluster size distribution and over the laser intensity distribution of a spatial Gaussian beam, which constitutes either a two-dimensional (2D) or a three-dimensional (3D) profile, with the 3D profile (when the cluster beam radius is larger than the Rayleigh length) usually being experimentally realized. The general features of the doubly averaged KEDs manifest the smearing out of the structure corresponding to the distribution of ion charges, a marked increase of the KEDs at very low energies due to the contribution from the persistent nanoplasma, a distortion of the KEDs and of the average energies toward lower energy values, and the appearance of long low-intensity high-energy tails caused by the admixture of contributions from large clusters by size averaging. The doubly averaged simulation results account reasonably well (within 30%) for the experimental data for the cluster-size dependence of the CE energetics and for its dependence on the laser pulse parameters, as well as for the anisotropy in the angular distribution of the energies of the Xe(q+) ions. Possible applications of this computational study include a control of the ion kinetic energies by the choice of the laser intensity profile (2D∕3D) in the laser-cluster interaction volume.
我们报告了在由超强度、近红外、高斯激光场(峰值强度为 10(15) - 4 × 10(16) W cm(-2),脉冲长度为 65-230 fs)驱动的元素 Xe(n) 团簇(平均尺寸 (n) = 200-2171)的库仑爆炸 (CE) 中,多电荷、高能离子的动能分布(KED)函数的计算。在这个团簇尺寸和脉冲参数范围内,外电离是不完全/垂直的、不完全/非垂直的或完全/非垂直的,在存在纳米等离子体电子的情况下会发生 CE。KED 是通过对单轨迹分子动力学模拟离子动能进行双平均获得的。KED 是在对数正态分布的团簇尺寸分布和空间高斯光束的激光强度分布上进行双重平均的,这构成了二维(2D)或三维(3D)轮廓,其中 3D 轮廓(当团簇束半径大于瑞利长度时)通常在实验中实现。双平均后的 KED 的一般特征表现为与离子电荷分布相对应的结构模糊化,由于Persistent Nanoplasma 的贡献,KED 在非常低的能量下显著增加,KED 和平均能量向较低能量值的扭曲,以及由于尺寸平均化导致的大团簇贡献的混合而出现的长而低强度的高能尾巴。双平均后的模拟结果很好地解释了(在 30%以内)CE 动力学的团簇尺寸依赖性以及其对激光脉冲参数的依赖性的实验数据,以及 Xe(q+)离子能量的角分布的各向异性。这项计算研究的可能应用包括通过选择激光-团簇相互作用体积中的激光强度分布(2D/3D)来控制离子动能。