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强场激发下过渡金属氧化物团簇中观察到的非定域电子行为。

Delocalized electronic behavior observed in transition metal oxide clusters under strong-field excitation.

机构信息

Departments of Chemistry and Physics, The Pennsylvania State University, University Park, Pennsylvania 16802, USA.

出版信息

J Chem Phys. 2011 Aug 7;135(5):054312. doi: 10.1063/1.3617231.

Abstract

Heterogeneously composed clusters are exposed to intensity resolved, 100 fs laser pulses to reveal the energy requirements for the production of the high charge states of both metal and nonmetal ions. The ionization and fragmentation of group V transition metal oxide clusters are here examined with laser intensities ranging nearly four orders in magnitude (∼3 × 10(11) W/cm(2) to ∼2 × 10(15) W/cm(2)) at 624 nm. The ionization potentials of the metal atoms are measured using both multiphoton ionization and tunneling ionization models. We demonstrate that the intensity selective scanning method can be utilized to measure the low ionization potentials of transition metals (∼7 eV). The high charge states demonstrate an enhancement in ionization that is three orders of magnitude lower in laser intensity than predicted for the atomic counterparts. Finally, the response from the various metals and the oxygen is compared to elucidate the mechanism of enhanced ionization that is observed. Specifically, the sequence of ion appearances demonstrates delocalized electron behavior over the entire cluster.

摘要

非均匀组成的团簇暴露在强度分辨的 100fs 激光脉冲下,以揭示产生金属和非金属离子高电荷态所需的能量。这里研究了激光强度范围近四个数量级(约 3×10(11)W/cm(2)至 2×10(15)W/cm(2))时 V 族过渡金属氧化物团簇的电离和碎裂,在 624nm 处。使用多光子电离和隧道电离模型测量了金属原子的电离势。我们证明,强度选择性扫描方法可用于测量过渡金属的低电离势(约 7eV)。高电荷态的电离增强程度比原子对应物的预测值低三个数量级,激光强度要低得多。最后,比较了各种金属和氧的响应,以阐明观察到的增强电离的机制。具体而言,离子出现的顺序表明整个团簇中的电子行为是离域的。

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