Reaction dynamics of the chimeric channelrhodopsin C1C2.
Reaction dynamics of the chimeric channelrhodopsin C1C2.
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DOI：
10.1038/s41598-017-07363-w
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发表时间：
2017-08-03
影响因子：
4.6
通讯作者：
Kennis JTM
中科院分区：
文献类型：
--
作者：
Hontani Y;Marazzi M;Stehfest K;Mathes T;van Stokkum IHM;Elstner M;Hegemann P;Kennis JTM
通道视紫红质(ChR)是光遗传工具包的关键蛋白。C1C2是莱茵衣藻ChR1和ChR2的功能性嵌合蛋白，是唯一一个晶体结构已被解决的CHR，因此非常适合于基于结构的分析。我们报道了超快瞬时吸收和多脉冲光谱结合靶分析和基于结构的量子力学/分子力学混合计算的C1C2光反应动力学。通过顺时针和逆时针旋转，在激发态(S1)上存在两条弛豫路径：(I)C13=C14异构化路径，经Cl1为450fs；(Ii)通过Cl2到达初始基态的驰豫路径为2.0 ps和11 ps，这取决于氢键网络，从而表明活性中心结构的异质性。额外的锥形交叉点Cl2的存在使相对较低的光异构化量子产率(30 ± 3%)合理化。此外，我们还展示了从皮秒到秒的光反应动力学，表征了C1C2的完整光循环。
Channelrhodopsin (ChR) is a key protein of the optogenetic toolkit. C1C2, a functional chimeric protein of Chlamydomonas reinhardtii ChR1 and ChR2, is the only ChR whose crystal structure has been solved, and thus uniquely suitable for structure-based analysis. We report C1C2 photoreaction dynamics with ultrafast transient absorption and multi-pulse spectroscopy combined with target analysis and structure-based hybrid quantum mechanics/molecular mechanics calculations. Two relaxation pathways exist on the excited (S1) state through two conical intersections CI1 and CI2, that are reached via clockwise and counter-clockwise rotations: (i) the C13=C14 isomerization path with 450 fs via CI1 and (ii) a relaxation path to the initial ground state with 2.0 ps and 11 ps via CI2, depending on the hydrogen-bonding network, hence indicating active-site structural heterogeneity. The presence of the additional conical intersection CI2 rationalizes the relatively low quantum yield of photoisomerization (30 ± 3%), reported here. Furthermore, we show the photoreaction dynamics from picoseconds to seconds, characterizing the complete photocycle of C1C2.
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影响因子：
62.1
作者：
Ernst, Oliver P.;Lodowski, David T.;Elstner, Marcus;Hegemann, Peter;Brown, Leonid S.;Kandori, Hideki
通讯作者：
Kandori, Hideki
影响因子：
13.9
作者：
Fenno L;Yizhar O;Deisseroth K
通讯作者：
Deisseroth K
影响因子：
16.6
作者：
Kato, Hideaki E.;Kamiya, Motoshi;Sugo, Seiya;Ito, Jumpei;Taniguchi, Reiya;Orito, Ayaka;Hirata, Kunio;Inutsuka, Ayumu;Yamanaka, Akihiro;Maturana, Andres D.;Ishitani, Ryuichiro;Sudo, Yuki;Hayashi, Shigehiko;Nureki, Osamu
通讯作者：
Nureki, Osamu
影响因子：
2.8
作者：
Blanco-Lomas, Marina;Campos, Pedro J.;Sampedro, Diego
通讯作者：
Sampedro, Diego
影响因子：
25
作者：
Boyden, ES;Zhang, F;Deisseroth, K
通讯作者：
Deisseroth, K