Isomerization mechanism of the HcRed fluorescent protein chromophore | |
Sun, Qiao1; Li, Zhen2; Lan, Zhenggang3,4; Pfisterer, Christoph5; Doerr, Markus3,6,7; Fischer, Stefan5; Smith, Sean C.1,8; Thiel, Walter3 | |
2012 | |
发表期刊 | PHYSICAL CHEMISTRY CHEMICAL PHYSICS |
卷号 | 14期号:32页码:11413-11424 |
摘要 | To understand how the protein achieves fluorescence, the isomerization mechanism of the HcRed chromophore is studied both under vacuum and in the solvated red fluorescent protein. Quantum mechanical (QM) and quantum mechanical/molecular mechanical (QM/MM) methods are applied both for the ground and the first excited state. The photoinduced processes in the chromophore mainly involve torsions around the imidazolinone-bridge bond (τ) and the phenoxy-bridge bond (φ). Under vacuum, the isomerization of the cis-trans chromophore essentially proceeds by τ twisting, while the radiationless decay requires φ torsion. By contrast, the isomerization of the cis-trans chromophore in HcRed occurs via simultaneous τ and φ twisting. The protein environment significantly reduces the barrier of this hula twist motion compared with vacuum. The excited-state isomerization barrier via the φ rotation of the cis-coplanar conformer in HcRed is computed to be significantly higher than that of the trans-non-coplanar conformer. This is consistent with the experimental observation that the cis-coplanar-conformation of the chromophore is related to the fluorescent properties of HcRed, while the trans-non-planar conformation is weakly fluorescent or non-fluorescent. Our study shows how the protein modifies the isomerization mechanism, notably by interactions involving the nearby residue Ile197, which keeps the chromophore coplanar and blocks the twisting motion that leads to photoinduced radiationless decay. |
文章类型 | Article |
学科领域 | 仿真与模拟 |
WOS标题词 | Science & Technology ; Physical Sciences |
DOI | 10.1039/c2cp41217a |
关键词[WOS] | PHOTOINDUCED NONADIABATIC DYNAMICS ; ELECTRONIC-STRUCTURE CALCULATIONS ; 2ND-ORDER PERTURBATION-THEORY ; PHOTOACTIVE YELLOW PROTEIN ; DENSITY-FUNCTIONAL THEORY ; SEMIEMPIRICAL METHODS ; MOLECULAR-DYNAMICS ; CRYSTAL-STRUCTURE ; PROTON-TRANSFER ; STRUCTURAL BASIS |
收录类别 | SCI |
语种 | 英语 |
WOS研究方向 | Chemistry ; Physics |
WOS类目 | Chemistry, Physical ; Physics, Atomic, Molecular & Chemical |
WOS记录号 | WOS:000306708300020 |
引用统计 | |
文献类型 | 期刊论文 |
条目标识符 | http://ir.qibebt.ac.cn/handle/337004/1312 |
专题 | 蛋白质设计研究组 |
作者单位 | 1.Univ Queensland, Ctr Computat Mol Sci, Australian Inst Bioengn & Nanotechnol, Brisbane, Qld 4072, Australia 2.Univ Wollongong, ISEM, Wollongong, NSW 2500, Australia 3.Max Planck Inst Kohlenforsch, D-45470 Mulheim, Germany 4.Chinese Acad Sci, Qingdao Inst Bioenergy & Bioproc Technol, Qingdao 266101, Peoples R China 5.Univ Heidelberg, IWR, D-69120 Heidelberg, Germany 6.Univ Santo Tomas, Fac Quim Ambiental, Bucaramanga, Colombia 7.Univ Ind Santander, Escuela Quim, Grp Bioquim Teor, Bucaramanga, Colombia 8.Oak Ridge Natl Lab, Ctr Nanophase Mat Sci, Oak Ridge, TN 37831 USA |
推荐引用方式 GB/T 7714 | Sun, Qiao,Li, Zhen,Lan, Zhenggang,et al. Isomerization mechanism of the HcRed fluorescent protein chromophore[J]. PHYSICAL CHEMISTRY CHEMICAL PHYSICS,2012,14(32):11413-11424. |
APA | Sun, Qiao.,Li, Zhen.,Lan, Zhenggang.,Pfisterer, Christoph.,Doerr, Markus.,...&Thiel, Walter.(2012).Isomerization mechanism of the HcRed fluorescent protein chromophore.PHYSICAL CHEMISTRY CHEMICAL PHYSICS,14(32),11413-11424. |
MLA | Sun, Qiao,et al."Isomerization mechanism of the HcRed fluorescent protein chromophore".PHYSICAL CHEMISTRY CHEMICAL PHYSICS 14.32(2012):11413-11424. |
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