2D IR spectroscopy of histidine: probing side-chain structure and dynamics via backbone amide vibrations.
2D IR spectroscopy of histidine: probing side-chain structure and dynamics via backbone amide vibrations.
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DOI：
10.1021/jp411901m
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发表时间：
2014-07-17
期刊：
影响因子：
--
通讯作者：
Gai F
中科院分区：
文献类型：
--
作者：
Ghosh A;Tucker MJ;Gai F
众所周知，组氨酸由于其侧链结构的多功能性而参与许多生物学功能。然而，探测蛋白质中组氨酸的构象转变，特别是那些发生在超快时间尺度上的构象转变是困难的。本文以组氨酸二肽为模型，通过测量其酰胺I振动跃迁的二维红外光谱，可以探测组氨酸残基的互变异构体和质子化状态。具体来说，对于所研究的组氨酸二肽，组氨酸的酰胺单元分别在大约1630、1644和1656 cm-1处产生三个光谱可分辨的酰胺I特征，根据不同pH值和频率计算，它们被分配给τ互变异构体（1630 cm-1成分）和π互变异构体（1644 cm-1成分）或脱水（1656 cm-1成分）酰胺。由于二维红外光谱固有的超快时间分辨率，我们相信当前的方法，当与同位素编辑技术相结合时，将有助于揭示蛋白质中对功能重要的关键组氨酸残基的结构动力学。
It is well known that histidine is involved in many biological functions due to the structural versatility of its side chain. However, probing the conformational transitions of histidine in proteins, especially those occurring on an ultrafast time scale, is difficult. Herein we show, using a histidine dipeptide as a model, that it is possible to probe the tautomer and protonation status of a histidine residue by measuring the two-dimensional infrared (2D IR) spectrum of its amide I vibrational transition. Specifically, for the histidine dipeptide studied, the amide unit of the histidine gives rise to three spectrally resolvable amide I features at approximately 1630, 1644, and 1656 cm–1, respectively, which, based on measurements at different pH values and frequency calculations, are assigned to a τ tautomer (1630 cm–1 component) and a π tautomer with a hydrated (1644 cm–1 component) or dehydrated (1656 cm–1 component) amide. Because of the intrinsic ultrafast time resolution of 2D IR spectroscopy, we believe that the current approach, when combined with the isotope editing techniques, will be useful in revealing the structural dynamics of key histidine residues in proteins that are important for function.
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DOI：
10.1126/science.1202997
发表时间：
2011-06-03
期刊：
Science (New York, N.Y.)
影响因子：
--
作者：
Remorino A;Korendovych IV;Wu Y;DeGrado WF;Hochstrasser RM
通讯作者：
Hochstrasser RM
DOI：
10.1021/jz301706a
发表时间：
2012-10-24
期刊：
The journal of physical chemistry letters
影响因子：
--
作者：
Peng CS;Tokmakoff A
通讯作者：
Tokmakoff A
影响因子：
3.3
作者：
Falvo, Cyril;Zhuang, Wei;Kim, Yung Sam;Axelsen, Paul H.;Hochstrasser, Robin M.;Mukamel, Shaul
通讯作者：
Mukamel, Shaul
影响因子：
15
作者：
Hass, Mathias A. S.;Hansen, D. Flemming;Kay, Lewis E.
通讯作者：
Kay, Lewis E.
来自固态NMR的流感M2质子通道中质子传导和门控的机制。
DOI：
10.1126/science.1191714
发表时间：
2010-10-22
期刊：
Science (New York, N.Y.)
影响因子：
--
作者：
Hu F;Luo W;Hong M
通讯作者：
Hong M