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非绝热电荷局域化辅助的大型多原子分子库仑爆炸

Coulomb explosion of large polyatomic molecules assisted by nonadiabatic charge localization.

作者信息

Markevitch Alexei N, Romanov Dmitri A, Smith Stanley M, Levis Robert J

机构信息

Department of Chemistry, Center for Advanced Photonics Research, Temple University, Philadelphia, Pennsylvania 19122, USA.

出版信息

Phys Rev Lett. 2004 Feb 13;92(6):063001. doi: 10.1103/PhysRevLett.92.063001. Epub 2004 Feb 12.

Abstract

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.

摘要

利用产生的H⁺离子的动能分布,对大型多原子分子蒽的库仑爆炸中的电子 - 核动力学进行了探测。对于暴露在强度为10¹⁴ W cm⁻²、持续时间为60 fs、波长800 nm的脉冲下的蒽, ejected质子的动能释放超过30 eV。我们基于(多次)电离分子中电荷分布的非绝热动力学提出了一个强场电荷局域化模型;电荷局域化持续许多激光周期,并通过分子离子的连续电离得以维持。该模型定量地解释了H⁺动能对激光强度的依赖性。由长寿命电荷局域化实现的多原子分子的解离电离是一种新型的电子 - 核动力学,对于理解强场中分子或离子碎片化的途径至关重要。

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