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Non-Adiabatic Molecular Dynamics Simulations of Non-Charge-Transfer and Charge-Transfer Scattering in H++CO2 at ELab=30 eV
Yun-An Yan,Jorge A. Morales*
Author NameAffiliationE-mail
Yun-An Yan Guizhou Provincial Key Laboratory of Computational Nano-material Science Guizhou Education University, Guiyang 550018, China  
Jorge A. Morales* Department of Chemistry and Biochemistry, Texas Tech University, PO Box 41061, Lubbock, TX 79409-1061, USA jorge.morales@ttu.edu 
Abstract:
The H++CO2 reaction at high energies is relevant in atmospheric chemistry, astrophysics, and proton cancer therapy research. Therefore, we present herein a complete investigation of H++CO2 at ELab=30 eV with the simplest-level electron nuclear dynamics (SLEND) method. SLEND describes nuclei via classical mechanics and electrons with a singledeterminantal Thouless wavefunction. The 3402 SLEND conducted simulations from 42 independent CO2 target orientations provide a full description of all the reactive processes and their mechanisms in this system:non-charge-transfer scattering (NCTS), charge-transfer scattering (CTS), and single C=O bond dissociation; all this valuable information about reactivity is not accessible experimentally. Numerous details of the projectile scattering patterns are provided, including the appearance and coalescence of primary and secondary rainbow angles as a function of the target orientation. SLEND NCTS and CTS differential cross sections (DCSs) are evaluated in conjunction with advanced semi-classical techniques. SLEND NCTS DCS agrees well with its experimental counterpart at all the measured scattering angles, whereas SLEND CTS DCS agrees well at high scattering angles but less satisfactorily at lower ones. Remarkably, both NCTS and CTS SLEND DCSs predict the primary rainbow angle signatures in agreement with the experiment.
Key words:  Quantum non-adiabatic dynamics  Proton-molecule reactions  Chargetransfer reactions  Primary and secondary rainbow angle effects  Collision-induced bond breaking  Proton cancer therapy
FundProject:Morales acknowledges financial support from the Cancer Prevention and Research Institute of Texas (CPRIT) grant RP140478. Prof. Yan acknowledges the financial support from the National Natural Science Foundation of China (No.21373064) and the Program for Innovative Research Team of Guizhou Province (No.QKTD[2014]4021).
H++CO2散射在30电子伏能量下电荷转移和非电荷转移的非绝热分子动力学模拟
严运安,Jorge A. Morales*
摘要:
在大气化学、天体物理学和癌症质子疗法中都涉及到高能H++CO2散射反应.本文在最简电子-核动力学(SLEND)基础上系统研究在30 eV下的H++CO2散射.SLEND用经典力学描述核,用单行列式Thouless波函数描述电子.本文模拟了CO2在42个取向共3402条轨线,为理解H++CO2散射中的各个反应过程和机制提供了系统描述:非电荷转移散射(NCTS),电荷转移散射(CTS)和C=O双键的断裂,这些关于反应的有用信息不能完全从实验中获取.本文提供了散射的详尽细节,包括随CO2取向不同主彩虹角和次彩虹角的出现和合并.SLEND NCTS和CTS的微分散射截面通过高等半经典方法计算,显示NCTS散射截面对所有散射角都同实验符合得很好,而CTS散射截面只大散射角时同实验结果符合得很好而在小角散射时稍差.无论是CTS还是NCTS SLEND都预言了主彩虹角的特征,这同实验完全一致.
关键词:  量子非绝热动力学  质子-分子反应  电荷转移反应  主和次彩虹角效应  碰撞诱导的化学键断裂  癌症质子疗法
DOI:10.1063/1674-0068/31/cjcp1712242
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