物理化学学报 >> 2008, Vol. 24 >> Issue (08): 1451-1458.doi: 10.3866/PKU.WHXB20080821

研究论文 上一篇    下一篇

分子动力学模拟纳米尺寸限制体系下氩溶液中I2的振动能量弛豫

毛荣荣; 吕洋; 周立川; 李钦宁; 李慎敏   

  1. 大连大学, 辽宁省生物有机重点实验室, 辽宁 大连 116622
  • 收稿日期:2008-02-26 修回日期:2008-04-30 发布日期:2008-08-06
  • 通讯作者: 李慎敏 E-mail:shenmin@dl.cn

Molecular Dynamics Simulation of the Vibrational Energy Relaxation of I2 in Nano-confined Argon Solution

MAO Rong-Rong; LV Yang; ZHOU Li-Chuan; LI Qin-Ning; LI Shen-Min   

  1. Liaoning Key Laboratory of Bioorganic Chemistry, Dalian University, Dalian 116622, Liaoning Province, P. R. China
  • Received:2008-02-26 Revised:2008-04-30 Published:2008-08-06
  • Contact: LI Shen-Min E-mail:shenmin@dl.cn

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摘要： 利用平衡态分子动力学方法(EMD)模拟了纳米尺寸限制球壳内I2在Ar溶液中的振动能量转移. 计算并讨论了I2振动能量弛豫时间T1随球壳半径、溶剂密度的变化规律. 通过分子间相互作用分析, 在原子、分子水平上, 揭示了随着球壳半径的减小, T1呈逐渐增大趋势的原因. 结果表明, 球壳的几何限制效应和表面作用对受限溶液密度分布的影响较大, 从而导致溶质振动弛豫的显著变化. 此外, 非限制体系模拟显示, 非平衡态分子动力学(NEMD)方法可以得到与平衡态分子动力学方法较一致的振动能量弛豫时间T1.

关键词: 纳米限制溶液, 平衡态分子动力学, 振动能量弛豫时间, 径向密度分布, 非平衡态分子动力学

Abstract: The vibrational energy transfer of I2 in argon solution confined in a nano-spherical cavity has been simulated by the equilibriummolecular dynamics (EMD) approach. The solute vibrational energy relaxation time T1, as a function of the radius of the spherical cavity and the solvent density, is calculated and discussed. According to the analysis of intermolecular interactions at atomic and molecular level, the reason of T1 increasing with the cavity radius decreasing is explored. The results showed that the geometry confinement and surface effect played an important role in the solvent distribution, which would influence the vibrational relaxation significantly. In addition, the simulations of bulk system indicated the values of T1 obtained by EMD and non-equilibrium molecular dynamics (NEMD)
were in good agreement for I2/Ar system.

Key words: Nano-confined solution, Equilibriummolecular dynamics, Vibrational energy relaxation time, Radial density distribution, Non-equilibriummolecular dynamics