GSTDTAP  > 地球科学
DOI10.1073/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
ISSN0027-8424
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
被引频次:19[WOS]   [WOS记录]     [WOS相关记录]
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.
条目包含的文件
条目无相关文件。
个性服务
推荐该条目
保存到收藏夹
查看访问统计
导出为Endnote文件
谷歌学术
谷歌学术中相似的文章
[Ajay, Jayanth S.]的文章
[Komarova, Ksenia G.]的文章
[Remacle, Francoise]的文章
百度学术
百度学术中相似的文章
[Ajay, Jayanth S.]的文章
[Komarova, Ksenia G.]的文章
[Remacle, Francoise]的文章
必应学术
必应学术中相似的文章
[Ajay, Jayanth S.]的文章
[Komarova, Ksenia G.]的文章
[Remacle, Francoise]的文章
相关权益政策
暂无数据
收藏/分享
所有评论 (0)
暂无评论
 

除非特别说明,本系统中所有内容都受版权保护,并保留所有权利。