Critical appraisal of excited state nonadiabatic dynamics simulations of 9H-adenine

doi:10.1063/1.4731649

QIBEBT-IR > 蛋白质设计研究组

	Critical appraisal of excited state nonadiabatic dynamics simulations of 9H-adenine
	Barbatti, Mario 1; Lan, Zhenggang 2; Crespo-Otero, Rachel 1; Szymczak, Jaroslaw J.3,4; Lischka, Hans 4,5; Thiel, Walter 1
	2012-12-14
发表期刊	JOURNAL OF CHEMICAL PHYSICS
卷号	137 期号:22
摘要	In spite of the importance of nonadiabatic dynamics simulations for the understanding of ultrafast photo-induced phenomena, simulations based on different methodologies have often led to contradictory results. In this work, we proceed through a comprehensive investigation of on-the-fly surface-hopping simulations of 9H-adenine in the gas phase using different electronic structure theories (ab initio, semi-empirical, and density functional methods). Simulations that employ ab initio and semi-empirical multireference configuration interaction methods predict the experimentally observed ultrafast deactivation of 9H-adenine with similar time scales, however, through different internal conversion channels. Simulations based on time-dependent density functional theory with six different hybrid and range-corrected functionals fail to predict the ultrafast deactivation. The origin of these differences is analyzed by systematic calculations of the relevant reaction pathways, which show that these discrepancies can always be traced back to topographical features of the underlying potential energy surfaces. (C) 2012 American Institute of Physics. [http://dx.doi.org/10.1063/1.4731649]
文章类型	Article
WOS标题词	Science & Technology ; Physical Sciences
DOI	10.1063/1.4731649
关键词[WOS]	RESOLVED PHOTOELECTRON-SPECTROSCOPY ; MULTICONFIGURATIONAL PERTURBATION-THEORY ; CONFIGURATION-INTERACTION METHODS ; ELECTRONIC RELAXATION DYNAMICS ; 3-STATE CONICAL INTERSECTIONS ; INITIO MOLECULAR-DYNAMICS ; DENSITY-FUNCTIONAL THEORY ; UNITARY-GROUP APPROACH ; NUCLEIC-ACID BASES ; AB-INITIO
收录类别	SCI
语种	英语
WOS研究方向	Physics
WOS类目	Physics, Atomic, Molecular & Chemical
WOS记录号	WOS:000312491400004
引用统计
文献类型	期刊论文
条目标识符	http://ir.qibebt.ac.cn/handle/337004/6063
专题	蛋白质设计研究组
作者单位	1.Max Planck Inst Kohlenforsch, D-45470 Mulheim, Germany 2.Chinese Acad Sci, Qingdao Inst Bioenergy & Bioproc Technol, Qingdao 266101, Peoples R China 3.Univ Basel, Dept Chem, CH-4056 Basel, Switzerland 4.Univ Vienna, Inst Theoret Chem, A-1090 Vienna, Austria 5.Texas Tech Univ, Dept Chem & Biochem, Lubbock, TX 79409 USA
推荐引用方式 GB/T 7714	Barbatti, Mario,Lan, Zhenggang,Crespo-Otero, Rachel,et al. Critical appraisal of excited state nonadiabatic dynamics simulations of 9H-adenine[J]. JOURNAL OF CHEMICAL PHYSICS,2012,137(22).
APA	Barbatti, Mario,Lan, Zhenggang,Crespo-Otero, Rachel,Szymczak, Jaroslaw J.,Lischka, Hans,&Thiel, Walter.(2012).Critical appraisal of excited state nonadiabatic dynamics simulations of 9H-adenine.JOURNAL OF CHEMICAL PHYSICS,137(22).
MLA	Barbatti, Mario,et al."Critical appraisal of excited state nonadiabatic dynamics simulations of 9H-adenine".JOURNAL OF CHEMICAL PHYSICS 137.22(2012).