Ultrafast Structural Dynamics of Biomolecules Examined by Multiple-Mode 2D IR Spectroscopy: Anharmonically Coupled Motions are in Harmony

doi:10.1002/cphc.200900301

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	Ultrafast Structural Dynamics of Biomolecules Examined by Multiple-Mode 2D IR Spectroscopy: Anharmonically Coupled Motions are in Harmony
	Wang, Jianping 1; Cai, Kaicong 1,2; Ma, Xiaoyan 1,2
刊名	CHEMPHYSCHEM
	2009-09-09
卷号	10 期号:13 页码:2242-2250
关键词	Ab Initio Calculations Biomolecules Ir Spectroscopy Molecular Dynamics Quantum Chemistry
ISSN号	1439-4235
DOI	10.1002/cphc.200900301
英文摘要	Quantum chemical computations, molecular dynamics simulations, and linear and nonlinear infrared spectral simulations are carried out for four representative biomolecules: cellobiose, alanine tripeptide, L-alpha-glycerylphosphorylethanolamine, and the DNA base monomer guanine. Anharmonic transition frequencies and anharmonicities for the molecules in vacuum are evaluated. Instantaneous normal-mode analysis is performed and the vibrational frequency distribution correlations are examined for the molecules solvated in TIP3P water. Many local and regional motions of the biomolecules are predicted to be anharmonically coupled and their vibrational frequencies are predicted to be largely correlated. These coupled and correlated vibrational motions can be easily visualized by cross peaks in the femtosecond broadband two-dimensional infrared (2D IR) spectra, which are simulated using time-domain third-order nonlinear response functions. A network of distinctive spectral profiles of the 2D IR cross peaks, including peak orientations and positive and negative signal patterns, are shown to be intimately connected with the couplings and correlations. The results show that the vibrational couplings and correlations, driven by solvent interactions and also by intrinsic vibrational interactions, are vibrational mode dependent and thus chemical group dependent, and form the structural and dynamical basis of the anharmonic vibrators that are ubiquitous in biomolecules.
语种	英语
出版者	WILEY-V C H VERLAG GMBH
WOS记录号	WOS:000269979600014
内容类型	期刊论文
源URL	[http://ir.iccas.ac.cn/handle/121111/66855]
专题	中国科学院化学研究所
通讯作者	Wang, Jianping
作者单位	1.Chinese Acad Sci, Beijing Natl Lab Mol Sci, State Key Lab Mol React Dynam, Inst Chem, Beijing 100190, Peoples R China 2.Chinese Acad Sci, Grad Sch, Beijing 100049, Peoples R China
推荐引用方式 GB/T 7714	Wang, Jianping,Cai, Kaicong,Ma, Xiaoyan. Ultrafast Structural Dynamics of Biomolecules Examined by Multiple-Mode 2D IR Spectroscopy: Anharmonically Coupled Motions are in Harmony[J]. CHEMPHYSCHEM,2009,10(13):2242-2250.
APA	Wang, Jianping,Cai, Kaicong,&Ma, Xiaoyan.(2009).Ultrafast Structural Dynamics of Biomolecules Examined by Multiple-Mode 2D IR Spectroscopy: Anharmonically Coupled Motions are in Harmony.CHEMPHYSCHEM,10(13),2242-2250.
MLA	Wang, Jianping,et al."Ultrafast Structural Dynamics of Biomolecules Examined by Multiple-Mode 2D IR Spectroscopy: Anharmonically Coupled Motions are in Harmony".CHEMPHYSCHEM 10.13(2009):2242-2250.