Controlling the strong field fragmentation of ClCHO+ using two laser pulses -an ab initio molecular dynamics simulation,Journal of Computational Chemistry

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Controlling the strong field fragmentation of ClCHO+ using two laser pulses -an ab initio molecular dynamics simulation
Journal of Computational Chemistry ( IF 3.4 ) Pub Date : 2018-10-14 , DOI: 10.1002/jcc.25576
Xuetao Shi ₁ , H. Bernhard Schlegel ₁

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For a single, intense 7 μm linearly polarized laser pulse, we found that the branching ratio for the fragmentation of ClCHO+ → Cl + HCO+, H + ClCO+, HCl++CO depended strongly on the orientation of the molecule (J. Phys. Chem. Lett. 2012, 3 2541). The present study explores the possibility of controlling the branching ratio for fragmentation by using two independent pulses with different frequencies, alignment and delay. Born‐Oppenheimer molecular dynamics simulations in the laser field were carried out with the B3LYP/6‐311G(d,p) level of theory using combinations of 3.5, 7 and 10.5 μm sine squared pulses with field strengths of 0.03 au (peak intensity of 3.15×1013 W/cm2) and lengths of 560 fs. A 3.5 μm pulse aligned with the C‐H bond and a 10.5 μm pulse perpendicular to the C‐H bond produced a larger branching ratio for HCl++CO than a comparable single 7 μm pulse. When the 10.5 μm pulse was delayed by one quarter of the pulse envelope, the branching ratio for the high energy product, (HCl++CO 73%) was a factor of three larger than the low energy product (Cl + HCO+, 25%). By contrast, when the 3.5 μm pulse was delayed by one quarter of the pulse envelope, the branching ratio was reversed (HCl++CO 38%; Cl + HCO+, 60%). Continuous wavelet analysis was used to follow the interaction of the laser with the various vibrational modes as a function of time. © 2018 Wiley Periodicals, Inc.

中文翻译：

使用两个激光脉冲控制 ClCHO+ 的强场碎裂——从头算分子动力学模拟

对于单个强 7 μm 线偏振激光脉冲，我们发现 ClCHO+ → Cl + HCO+、H + ClCO+、HCl++CO 的分裂分支比强烈依赖于分子的取向（J. Phys. Chem . Lett. 2012, 3 2541)。本研究探索了通过使用具有不同频率、对齐和延迟的两个独立脉冲来控制分裂的分支比的可能性。激光场中的 Born-Oppenheimer 分子动力学模拟是在 B3LYP/6-311G(d,p) 理论水平下使用 3.5、7 和 10.5 μm 正弦平方脉冲的组合进行的，场强为 0.03 au（峰值强度为3.15×1013 W/cm2) 和 560 fs 的长度。3.5 μm 脉冲与 C-H 键和 10. 与可比较的单个 7 μm 脉冲相比，垂直于 C-H 键的 5 μm 脉冲对 HCl++CO 产生更大的支化率。当 10.5 μm 脉冲延迟脉冲包络的四分之一时，高能产物 (HCl++CO 73%) 的分支比比低能产物 (Cl + HCO+, 25%) 大三倍）。相比之下，当 3.5 μm 脉冲延迟脉冲包络的四分之一时，分支比发生逆转（HCl++CO 38%；Cl + HCO+，60%）。连续小波分析用于跟踪激光与各种振动模式作为时间函数的相互作用。© 2018 Wiley Periodicals, Inc. (HCl++CO 73%) 是低能量产品 (Cl + HCO+, 25%) 的三倍。相比之下，当 3.5 μm 脉冲延迟脉冲包络的四分之一时，分支比发生逆转（HCl++CO 38%；Cl + HCO+，60%）。连续小波分析用于跟踪激光与各种振动模式作为时间函数的相互作用。© 2018 Wiley Periodicals, Inc. (HCl++CO 73%) 是低能量产品 (Cl + HCO+, 25%) 的三倍。相比之下，当 3.5 μm 脉冲延迟脉冲包络的四分之一时，分支比发生逆转（HCl++CO 38%；Cl + HCO+，60%）。连续小波分析用于跟踪激光与各种振动模式作为时间函数的相互作用。© 2018 Wiley Periodicals, Inc.

更新日期：2018-10-14

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