{"title":"分子内振动能量再分配与单分子解离之间的竞争:一个散射理论的观点","authors":"K. Someda, Hiroki Nakamura, F. Mies","doi":"10.1155/1995/59696","DOIUrl":null,"url":null,"abstract":"Systematic behavior of decay rates of resonances above dissociation threshold is investigated by using the theory of resonance scattering. The condition for the Rice-Ramsperger-Kassel-Marcus (RRKM) rate formula to be valid is clarified by analyzing the random model of unimolecular dissociation. The decay rate averaged over many resonances agrees with the RRKM rate when the mean spacing and the mean width of the resonance states coincide with each other. On the other hand, auto- and mutual-correlation functions of the non-stationary wave functions indicate a rather paradoxical and intriguing phenomenon: In the RRKM regime, insufficient time is left for intramolecular vibrational energy redistribution (IVR) before dissociation.","PeriodicalId":296295,"journal":{"name":"Laser Chemistry","volume":"145 1","pages":"0"},"PeriodicalIF":0.0000,"publicationDate":"1900-01-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":"3","resultStr":"{\"title\":\"Competition Between Intramolecular Vibrational Energy Re-Distribution and Unimolecular Dissociation: A Scattering Theoretical Point of View\",\"authors\":\"K. Someda, Hiroki Nakamura, F. Mies\",\"doi\":\"10.1155/1995/59696\",\"DOIUrl\":null,\"url\":null,\"abstract\":\"Systematic behavior of decay rates of resonances above dissociation threshold is investigated by using the theory of resonance scattering. The condition for the Rice-Ramsperger-Kassel-Marcus (RRKM) rate formula to be valid is clarified by analyzing the random model of unimolecular dissociation. The decay rate averaged over many resonances agrees with the RRKM rate when the mean spacing and the mean width of the resonance states coincide with each other. On the other hand, auto- and mutual-correlation functions of the non-stationary wave functions indicate a rather paradoxical and intriguing phenomenon: In the RRKM regime, insufficient time is left for intramolecular vibrational energy redistribution (IVR) before dissociation.\",\"PeriodicalId\":296295,\"journal\":{\"name\":\"Laser Chemistry\",\"volume\":\"145 1\",\"pages\":\"0\"},\"PeriodicalIF\":0.0000,\"publicationDate\":\"1900-01-01\",\"publicationTypes\":\"Journal Article\",\"fieldsOfStudy\":null,\"isOpenAccess\":false,\"openAccessPdf\":\"\",\"citationCount\":\"3\",\"resultStr\":null,\"platform\":\"Semanticscholar\",\"paperid\":null,\"PeriodicalName\":\"Laser Chemistry\",\"FirstCategoryId\":\"1085\",\"ListUrlMain\":\"https://doi.org/10.1155/1995/59696\",\"RegionNum\":0,\"RegionCategory\":null,\"ArticlePicture\":[],\"TitleCN\":null,\"AbstractTextCN\":null,\"PMCID\":null,\"EPubDate\":\"\",\"PubModel\":\"\",\"JCR\":\"\",\"JCRName\":\"\",\"Score\":null,\"Total\":0}","platform":"Semanticscholar","paperid":null,"PeriodicalName":"Laser Chemistry","FirstCategoryId":"1085","ListUrlMain":"https://doi.org/10.1155/1995/59696","RegionNum":0,"RegionCategory":null,"ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":null,"EPubDate":"","PubModel":"","JCR":"","JCRName":"","Score":null,"Total":0}
Competition Between Intramolecular Vibrational Energy Re-Distribution and Unimolecular Dissociation: A Scattering Theoretical Point of View
Systematic behavior of decay rates of resonances above dissociation threshold is investigated by using the theory of resonance scattering. The condition for the Rice-Ramsperger-Kassel-Marcus (RRKM) rate formula to be valid is clarified by analyzing the random model of unimolecular dissociation. The decay rate averaged over many resonances agrees with the RRKM rate when the mean spacing and the mean width of the resonance states coincide with each other. On the other hand, auto- and mutual-correlation functions of the non-stationary wave functions indicate a rather paradoxical and intriguing phenomenon: In the RRKM regime, insufficient time is left for intramolecular vibrational energy redistribution (IVR) before dissociation.
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