Last Isidore, Levy Yaakov, Jortner Joshua
School of Chemistry, Tel Aviv University, Ramat Aviv, 69978 Tel Aviv, Israel.
J Chem Phys. 2005 Oct 15;123(15):154301. doi: 10.1063/1.2052567.
We address unifying features of fragmentation channels driven by long-range Coulomb or pseudo-Coulomb forces in clusters, nuclei, droplets, and optical molasses. We studied the energetics, fragmentation patterns, and dynamics of multicharged (A+)n (n=55, 135, 321) clusters. In Morse clusters the variation of the range of the pair-potential induced changes in the cluster surface energy and in the fissibility parameter X=E(Coulomb)2E(surface). X was varied in the range of X=1-8 for short-range interactions and of X=0.1-1.0 for long-range interactions. Metastable cluster configurations were prepared by vertical ionization of the neutral clusters and by subsequent structural equilibration. The energetics of these metastable ionic clusters was described in terms of the liquid drop model, with the coefficients of the volume and surface energies depending linearly on the Morse band dissociation energy. Molecular-dynamics simulations established two distinct fragmentation patterns of multicharged clusters that involve cluster fission into a small number of large, multicharged clusters for X<1 and Coulomb explosion into a large number of individual ions and small ionic fragments for X>1. The Rayleigh instability limit X=1 separates between spatially anisotropic fission and spatially isotropic Coulomb explosion. Distinct features of the fragmentation energetics and dynamics were unveiled. For fission of n=55 clusters, large kinetic and internal energies of the large fragments are exhibited and the characteristic fragmentation time is approximately 700 fs, while for Coulomb explosion the major energy content of the small fragments involves kinetic energy and the characteristic fragmentation time of approximately 300 fs is shorter. The Rayleigh (X=1) limit, leading to isotropic Coulomb explosion, is transcended by a marked enhancement of the Coulomb energy, which is realized for extremely ionized clusters in ultraintense laser fields, or by a dramatic reduction of the surface energy as is the case for the expansion of optical molasses.
我们探讨了由长程库仑力或类库仑力驱动的团簇、原子核、液滴和光学糖浆中的碎裂通道的统一特征。我们研究了多电荷(A+)n(n = 55、135、321)团簇的能量学、碎裂模式和动力学。在莫尔斯团簇中,对势范围的变化会引起团簇表面能和裂变参数X = E(库仑)/2E(表面)的变化。对于短程相互作用,X在X = 1 - 8范围内变化,对于长程相互作用,X在X = 0.1 - 1.0范围内变化。通过中性团簇的垂直电离和随后的结构平衡制备亚稳团簇构型。这些亚稳离子团簇的能量学用液滴模型来描述,体积能和表面能的系数线性依赖于莫尔斯带解离能。分子动力学模拟确定了多电荷团簇的两种不同碎裂模式,对于X < 1,涉及团簇裂变为少数几个大的多电荷团簇,对于X > 1,涉及库仑爆炸为大量单个离子和小的离子碎片。瑞利不稳定性极限X = 1区分了空间各向异性裂变和空间各向同性库仑爆炸。揭示了碎裂能量学和动力学的独特特征。对于n = 55团簇的裂变,大碎片表现出较大的动能和内能,特征碎裂时间约为700飞秒,而对于库仑爆炸,小碎片的主要能量成分是动能,特征碎裂时间约为300飞秒,较短。导致各向同性库仑爆炸的瑞利(X = 1)极限,通过库仑能的显著增强而被超越,这在超强激光场中极度电离的团簇中实现,或者通过表面能的急剧降低,如光学糖浆膨胀的情况。