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超快强激光诱导的甲烷爆炸光解离

Explosive photodissociation of methane induced by ultrafast intense laser.

作者信息

Kong Fanao, Luo Qi, Xu Huailiang, Sharifi Mehdi, Song Di, Chin See Leang

机构信息

Institute of Chemistry, Chinese Academy of Sciences, Beijing 100080, People's Republic of China.

出版信息

J Chem Phys. 2006 Oct 7;125(13):133320. doi: 10.1063/1.2204919.

Abstract

A new type of molecular fragmentation induced by femtosecond intense laser at the intensity of 2 x 10(14) W/cm2 is reported. For the parent molecule of methane, ethylene, n-butane, and 1-butene, fluorescence from H (n = 3-->2), CH (A 2Delta, B 2Sigma-, and C 2Sigma+-->X 2Pi), or C2 (d 3Pi g-->a 3Pi u) is observed in the spectrum. It shows that the fragmentation is a universal property of neutral molecule in the intense laser field. Unlike breaking only one or two chemical bonds in conventional UV photodissociation, the fragmentation caused by the intense laser undergoes vigorous changes, breaking most of the bonds in the molecule, like an explosion. The fragments are neutral species and cannot be produced through Coulomb explosion of multiply charged ion. The laser power dependence of CH (A-->X) emission of methane on a log-log scale has a slope of 10 +/- 1. The fragmentation is thus explained as multiple channel dissociation of the superexcited state of parent molecule, which is created by multiphoton excitation.

摘要

报道了一种由强度为2×10¹⁴W/cm²的飞秒强激光诱导产生的新型分子碎片化现象。对于甲烷、乙烯、正丁烷和1-丁烯的母体分子,在光谱中观察到了来自H(n = 3→2)、CH(A²Δ、B²Σ⁻和C²Σ⁺→X²Π)或C₂(d³Πg→a³Πu)的荧光。这表明碎片化是强激光场中中性分子的一种普遍特性。与传统紫外光解离中仅断裂一两个化学键不同,强激光引起的碎片化会发生剧烈变化,断裂分子中的大部分化学键,就像爆炸一样。碎片是中性物种,不能通过多电荷离子的库仑爆炸产生。甲烷的CH(A→X)发射的激光功率对数-对数关系曲线的斜率为10±1。因此,这种碎片化被解释为母体分子超激发态的多通道解离,超激发态是由多光子激发产生的。

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