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PNAS Plus: Pendular alignment and strong chemical binding are induced in helium dimer molecules by intense laser fields

机译:PNAS Plus:强激光场在氦二聚体分子中诱导垂线排列和牢固的化学结合

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摘要

Intense pulsed-laser fields have provided means to both induce spatial alignment of molecules and enhance strength of chemical bonds. The duration of the laser field typically ranges from hundreds of picoseconds to a few femtoseconds. Accordingly, the induced “laser-dressed” properties can be adiabatic, existing only during the pulse, or nonadiabatic, persisting into the subsequent field-free domain. We exemplify these aspects by treating the helium dimer, in its ground (X1Σg+) and first excited (A1Σu+) electronic states. The ground-state dimer when field-free is barely bound, so very responsive to electric fields. We examine two laser realms, designated (I) “intrusive” and (II) “impelling.” I employs intense nonresonant laser fields, not strong enough to dislodge electrons, yet interact with the dimer polarizability to induce binding and pendular states in which the dimer axis librates about the electric field direction. II employs superintense high-frequency fields that impel the electrons to undergo quiver oscillations, which interact with the intrinsic Coulomb forces to form an effective binding potential. The dimer bond then becomes much stronger. For I, we map laser-induced pendular alignment within the X state, which is absent for the field-free dimer. For II, we evaluate vibronic transitions from the X to A states, governed by the amplitude of the quiver oscillations.
机译:强脉冲激光场提供了既诱导分子的空间排列并增强化学键强度的手段。激光场的持续时间通常在数百皮秒到几飞秒的范围内。因此,诱导的“激光修饰”特性可以是绝热的,仅在脉冲期间存在,或非绝热的,持续到随后的无场域中。我们通过在地面上处理氦二聚体来举例说明这些方面。 X 1 Σ g + 并首先兴奋 < mrow> A 1 < msubsup> Σ u + 电子状态。当没有电场时,基态二聚体几乎不受约束,因此对电场非常敏感。我们研究了两个激光领域,分别称为(I)“侵入式”和(II)“推动式”。我使用了强烈的非共振激光场,其强度不足以驱散电子,但仍与二聚体极化作用相互作用,以诱导二聚体轴围绕电场方向释放的结合和摆动状态。 II使用超强高频场,促使电子经历颤动振荡,颤动振荡与固有库仑力相互作用形成有效的结合势。然后,二聚体键变得更强。对于I,我们在X态内映射激光诱导的摆线对准,这对于无场二聚体是不存在的。对于II,我们评估了由颤动振幅控制的从X态到A态的振动跃迁。

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