Chemistry Division, Bhabha Atomic Research Center, Mumbai, 400 085, India.
J Am Soc Mass Spectrom. 2017 Nov;28(11):2361-2370. doi: 10.1007/s13361-017-1755-3. Epub 2017 Jul 21.
Systematic manipulation of ionic-outcome in laser-cluster interaction process has been realized for studies carried out on tetramethyltin (TMT) clusters under picosecond laser conditions, determined by choice of laser wavelength and intensity. As a function of laser intensity, TMT clusters exhibit gradual enhancement in overall ionization of its cluster constituents, up to a saturation level of ionization, which was distinct for different wavelengths (266, 355, and 532 nm). Simultaneously, systematic appearance of higher multiply charged atomic ions and shift in relative abundance of multiply charged atomic ions towards higher charge state was observed, using time-of-flight mass spectrometer. At saturation level, multiply charged atomic ions up to (C, Sn) at 266 nm, (C, Sn) at 355 nm, and (C, Sn) at 532 nm were detected. In addition, at 355 nm intra-cluster ion chemistry within the ionized cluster leads to generation of molecular hydrogen ion (H) and triatomic molecular hydrogen ion (H). Generation of multiply charged atomic ions is ascribed to efficient coupling of laser pulse with the cluster media, facilitated by inner-ionized electrons produced within the cluster, at the leading edge of laser pulse. Role of inner-ionized electrons is authenticated by measuring kinetic energy distribution of electrons liberated upon disintegration of excessively ionized cluster, under the influence of picosecond laser pulse. Graphical Abstract ᅟ.
在皮秒激光条件下对四甲基锡(TMT)团簇进行的研究中,通过选择激光波长和强度,实现了激光-团簇相互作用过程中离子产物的系统操纵。随着激光强度的变化,TMT 团簇表现出其团簇组成部分的总离化逐渐增强,直至达到离化的饱和水平,这对于不同的波长(266、355 和 532nm)是不同的。同时,使用飞行时间质谱仪观察到,随着激光强度的增加,多电荷原子离子的系统出现以及多电荷原子离子的相对丰度向更高电荷态的转移。在饱和水平下,在 266nm 时检测到(C, Sn)的多电荷原子离子,在 355nm 时检测到(C, Sn)的多电荷原子离子,在 532nm 时检测到(C, Sn)的多电荷原子离子。此外,在 355nm 时,在激光脉冲的前沿,离子化簇内的离子内化学导致产生氢离子(H)和三原子氢离子(H)。多电荷原子离子的产生归因于激光脉冲与团簇介质的有效耦合,这是由团簇内产生的内电离电子促成的。通过测量在皮秒激光脉冲的影响下,过度离化的团簇分解时释放的电子的动能分布,证实了内电离电子的作用。