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DOI | 10.1073/pnas.1804455115 |
Time-dependent view of an isotope effect in electron-nuclear nonequilibrium dynamics with applications to N-2 | |
Ajay, Jayanth S.1,2; Komarova, Ksenia G.1,2; Remacle, Francoise1,2,3; Levine, R. D.1,2,4,5 | |
2018-06-05 | |
发表期刊 | PROCEEDINGS OF THE NATIONAL ACADEMY OF SCIENCES OF THE UNITED STATES OF AMERICA |
ISSN | 0027-8424 |
出版年 | 2018 |
卷号 | 115期号:23页码:5890-5895 |
文章类型 | Article |
语种 | 英语 |
国家 | Israel; Belgium; USA |
英文摘要 | Isotopic fractionation in the photodissociation of N-2 could explain the considerable variation in the N-14/N-15 ratio in different regions of our galaxy. We previously proposed that such an isotope effect is due to coupling of photoexcited bound valence and Rydberg electronic states in the frequency range where there is strong state mixing. We here identify features of the role of the mass in the dynamics through a time-dependent quantum-mechanical simulation. The photoexcitation of N-2 is by an ultrashort pulse so that the process has a sharply defined origin in time and so that we can monitor the isolated molecule dynamics in time. An ultrafast pulse is necessarily broad in frequency and spans several excited electronic states. Each excited molecule is therefore not in a given electronic state but in a superposition state. A short time after excitation, there is a fairly sharp onset of amass-dependent large population transfer when wave packets on two different electronic states in the same molecule overlap. This coherent overlap of the wave packets on different electronic states in the region of strong coupling allows an effective transfer of population that is very mass dependent. The extent of the transfer depends on the product of the populations on the two different electronic states and on their relative phase. It is as if two molecules collide but the process occurs within one molecule, a molecule that is simultaneously in both states. An analytical toy model recovers the ( strong) mass and energy dependence. |
英文关键词 | diabatic electronic states nuclear phase electronic coherence photodissociation nonstationary states |
领域 | 地球科学 ; 气候变化 ; 资源环境 |
收录类别 | SCI-E |
WOS记录号 | WOS:000434114900038 |
WOS关键词 | POTENTIAL-ENERGY CURVES ; PREDISSOCIATION MECHANISM ; (1)PI(U) STATES ; ULTRAFAST ; PROBE |
WOS类目 | Multidisciplinary Sciences |
WOS研究方向 | Science & Technology - Other Topics |
URL | 查看原文 |
引用统计 | |
文献类型 | 期刊论文 |
条目标识符 | http://119.78.100.173/C666/handle/2XK7JSWQ/204928 |
专题 | 地球科学 资源环境科学 气候变化 |
作者单位 | 1.Hebrew Univ Jerusalem, Fritz Haber Ctr Mol Dynam, IL-91904 Jerusalem, Israel; 2.Hebrew Univ Jerusalem, Inst Chem, IL-91904 Jerusalem, Israel; 3.Univ Liege, Res Unit Mol Syst B6c, Theoret Phys Chem, B-4000 Liege, Belgium; 4.Univ Calif Los Angeles, David Geffen Sch Med, Dept Mol & Med Pharmacol, Los Angeles, CA 90095 USA; 5.Univ Calif Los Angeles, Dept Chem & Biochem, Los Angeles, CA 90095 USA |
推荐引用方式 GB/T 7714 | Ajay, Jayanth S.,Komarova, Ksenia G.,Remacle, Francoise,et al. Time-dependent view of an isotope effect in electron-nuclear nonequilibrium dynamics with applications to N-2[J]. PROCEEDINGS OF THE NATIONAL ACADEMY OF SCIENCES OF THE UNITED STATES OF AMERICA,2018,115(23):5890-5895. |
APA | Ajay, Jayanth S.,Komarova, Ksenia G.,Remacle, Francoise,&Levine, R. D..(2018).Time-dependent view of an isotope effect in electron-nuclear nonequilibrium dynamics with applications to N-2.PROCEEDINGS OF THE NATIONAL ACADEMY OF SCIENCES OF THE UNITED STATES OF AMERICA,115(23),5890-5895. |
MLA | Ajay, Jayanth S.,et al."Time-dependent view of an isotope effect in electron-nuclear nonequilibrium dynamics with applications to N-2".PROCEEDINGS OF THE NATIONAL ACADEMY OF SCIENCES OF THE UNITED STATES OF AMERICA 115.23(2018):5890-5895. |
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