2003 Fiscal Year Final Research Report Summary
Wavepacket dynamics of ultrafast reactions with relaxation
| Project/Area Number |
14340174
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| Research Category |
Grant-in-Aid for Scientific Research (B)
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| Allocation Type | Single-year Grants |
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| Section | 一般 |
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| Research Field |
Physical chemistry
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| Research Institution | The University of Tokyo |
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Principal Investigator |
YAMASHITA Koichi The University of Tokyo, School of Engineering, Professor, 大学院・工学系研究科, 教授 (40175659)
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| Co-Investigator(Kenkyū-buntansha) |
NAKAMURA Hisao The University of Tokyo, School of Engineering, Research Associate, 大学院・工学系研究科, 助手 (30345095)
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| Project Period (FY) |
2002 – 2003
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| Keywords | DIET / Photo-induced Dsorption / NO / Pt(111) system / vibrational excitation / energy dissipation Process / density matrix / cluster model / wavepacket dynamics |
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| Research Abstract |
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.
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