Wavepacket dynamics of ultrafast reactions with relaxation

弛豫超快反应的波包动力学

• 批准号: 14340174
• 负责人: YAMASHITA Koichi
• 金额: $ 8.64万
• 依托单位: The University of Tokyo
• 依托单位国家: 日本
• 项目类别: Grant-in-Aid for Scientific Research (B)
• 财政年份: 2002
• 资助国家: 日本
• 起止时间: 2002 至 2003
• 项目状态: 已结题
• 来源: https://kaken.nii.ac.jp/en/grant/KAKENHI-PROJECT-14340174/
• 关键词: DIET; Photo-induced Dsorption; NO; Pt(111) system; vibrational excitation; energy dissipation Process; density matrix; cluster model; wavepacket dynamics; 電子遷移誘起脱離; 光誘起脱離反応; 振動緩和; 超高速反応; 緩和過程; チャープパルス; レーザー制御; 密度行列法; 光脱離過程; 金属表面反応

The effect of vibrational relaxation on the photodesorption dynamics of NO from a Pt(111) surface has been investigated theoretically. Although this system has been studied in many previous works, the relaxation of NO stretching vibration due to the interaction with electron-hole pairs in metals has not been included in conventional models. Although the relaxation lifetimes of the first-excited vibrational state of diatomic molecules adsorbed on metal surfaces are generally in the range 0.1-1 ps, the desorption dynamics of NO complete in about 1 ps. Therefore, it is considered that the vibrational relaxation can influence the vibrational state of this stretching mode during the desorption process. We described the desorption dynamics by using the time propagation of the density matrix. The effects of vibrational relaxation were included by using a Redfleld-like model. We also investigated the validity of the parameters for dynamical calculations by ab initio methods. As a result, we obtained physically reasonable results for the desorption probability, the mean translational energy, and the vibrational state distribution for the desorbed NO molecules.

从理论上研究了NO在Pt（111）表面上的光脱附动力学过程中振动弛豫的影响。虽然这个系统已经在许多以前的工作中进行了研究，NO伸缩振动的弛豫由于与金属中的电子空穴对的相互作用还没有包括在传统的模型。虽然吸附在金属表面上的双原子分子的第一激发振动态的弛豫寿命通常在0.1-1 ps范围内，但NO的脱附动力学在约1 ps内完成。因此，可以认为，在脱附过程中，振动弛豫可以影响该伸缩模的振动状态。我们用密度矩阵的时间传播描述了脱附动力学。振动弛豫的影响，包括通过使用一个雷德菲尔德的模型。我们还研究了从头算方法的动力学计算参数的有效性。因此，我们得到了物理上合理的结果的脱附概率，平均平移能，和脱附NO分子的振动态分布。

项目成果

A.Abe, K.Yamashita: "Effects of Vibrational Relaxation on the Photodesorption of NO from Pt(111) : A Density Matrix Study"J.Chem.Phys.. 119. 9710-9718 (2003)

A.Abe、K.Yamashita：“振动弛豫对 Pt(111) 中 NO 光解吸的影响：密度矩阵研究”J.Chem.Phys.. 119. 9710-9718 (2003)

A.Abe, K.Yamashita: "Effects of Vibrational Relaxation on the Photodesorption of NO from Pt(1 11): A Density Matrix Study"J. Chem. Phys.. 119. 9710-9718 (2003)

A.Abe，K.Yamashita：“振动弛豫对 Pt(1 11) 中 NO 光解吸的影响：密度矩阵研究”J。

A.Abe: "A Wavepacket Study on Translational Energy Distributions of the Photo-stimulated Desorbed Xe from an Oxidaized Si(001)"Bull.Korean CHem.Soc.. 24. 691-694 (2003)

A.Abe：“氧化 Si(001) 中光刺激解吸 Xe 的平移能量分布的波包研究”Bull.Korean CHem.Soc.. 24. 691-694 (2003)

A.Abe: "Effects of vibrational relaxation on the photodesorption of NO from Pt(111) : A density Matrix Study"J.Chem.Phys.. 119. 9710-9718 (2003)

A.Abe：“振动弛豫对 Pt(111) 中 NO 光解吸的影响：密度矩阵研究”J.Chem.Phys.. 119. 9710-9718 (2003)

田中, 中島, 山下: "Density functional study on the reactivity Cl oxidized aluminium surfaces : effects of adsorbed metallic atoms"Thin Solid Films. 409. 66-73 (2002)

Tanaka、Nakajima、Yamashita：“Cl 氧化铝表面反应性的密度泛函研究：吸附金属原子的影响”薄固体薄膜。 409. 66-73 (2002)