中国科学院机构知识库网格
Chinese Academy of Sciences Institutional Repositories Grid
Photoinduced Charge Transfer versus Fragmentation Pathways in Lanthanum Cyclopentadienyl Complexes

文献类型:期刊论文

作者Han, Yulun; Rasulev, Bakhtiyor; May, P. Stanley; Berry, Mary T.; Kilin, Dmitri S.; Kilin, DS
刊名JOURNAL OF CHEMICAL THEORY AND COMPUTATION
出版日期2017
卷号13期号:9页码:4281-4296
ISSN号1549-9618
产权排序2
英文摘要

This study compares two competing pathways of photoexcitations in gas-phase metal organic complexes: first, a sequence of phonon-assisted electronic transitions leading to dissipation of the energy of photoexcitations and, second, a sequence of light-driven electronic transitions "leadingto photolysis. Phonon-assisted charge carrier dynamics is investigated by combination of the density matrix formalism and on-the-fly non adiabatic couplings. Light-driven fragmentation is modeled by a time-dependent excited-state molecular-dynamics (TDESMD) algorithm based on Rabi theory and principles similar to the trajectory surface hopping approximation. Numerical results indicate that, under the medium intensity of the laser field, light driven electronic transitions are more probable than phonon-assisted ones. The formation of multiple products is observed in TDESMD trajectories. Simulated mass spectra are extracted from TDESMD simulations and compared to experimental photoionization time-of-flight (PI-TOF) mass spectra. It is found that several features in the experimental mass spectra are reproduced by the simulations.

WOS关键词OXIDE THIN-FILMS ; ATOMIC LAYER DEPOSITION ; INITIO MOLECULAR-DYNAMICS ; CHEMICAL-VAPOR-DEPOSITION ; GENERALIZED GRADIENT APPROXIMATION ; GAS-PHASE PHOTOFRAGMENTATION ; MULTILEVEL REDFIELD THEORY ; COUPLED ELECTRON-TRANSFER ; DENSITY-FUNCTIONAL THEORY ; TOTAL-ENERGY CALCULATIONS
WOS研究方向Chemistry ; Physics
语种英语
WOS记录号WOS:000410867500030
资助机构NSF [EPS-0903804, CHE-1413614] ; DOE, BES-Chemical Sciences ; NERSC [DE-AC02-05CH11231, 91202] ; NDSU Department of Chemistry and Biochemistry and College of Science and Mathematics ; North Dakota State University Center ; U.S. Department of Energy [DE-SC0001717] ; National Science Foundation under ND EPSCoR [IIA-1355466] ; State of North Dakota
源URL[http://ir.sia.cn/handle/173321/20999]  
专题沈阳自动化研究所_广州中国科学院沈阳自动化研究所分所
作者单位1.Shenyang Institute of Automation, Guangzhou, Chinese Academy of Sciences, Guangzhou 511458, China
2.Department of Chemistry, University of South Dakota, Vermillion, South Dakota 57069, United States
3.Center for Computationally Assisted Science and Technology, North Dakota State University, Fargo, North Dakota 58102, United States
4.Department of Coatings and Polymeric Materials, North Dakota State University, Fargo, North Dakota 58102, United States
5.Department of Chemistry and Biochemistry, North Dakota State University, Fargo, North Dakota 58108, United States
推荐引用方式
GB/T 7714
Han, Yulun,Rasulev, Bakhtiyor,May, P. Stanley,et al. Photoinduced Charge Transfer versus Fragmentation Pathways in Lanthanum Cyclopentadienyl Complexes[J]. JOURNAL OF CHEMICAL THEORY AND COMPUTATION,2017,13(9):4281-4296.
APA Han, Yulun,Rasulev, Bakhtiyor,May, P. Stanley,Berry, Mary T.,Kilin, Dmitri S.,&Kilin, DS.(2017).Photoinduced Charge Transfer versus Fragmentation Pathways in Lanthanum Cyclopentadienyl Complexes.JOURNAL OF CHEMICAL THEORY AND COMPUTATION,13(9),4281-4296.
MLA Han, Yulun,et al."Photoinduced Charge Transfer versus Fragmentation Pathways in Lanthanum Cyclopentadienyl Complexes".JOURNAL OF CHEMICAL THEORY AND COMPUTATION 13.9(2017):4281-4296.

入库方式: OAI收割

来源:沈阳自动化研究所

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