Early-stage dynamics of chloride ion-pumping rhodopsin revealed by a femtosecond X-ray laser.
Early-stage dynamics of chloride ion-pumping rhodopsin revealed by a femtosecond X-ray laser.
复制标题
DOI：
10.1073/pnas.2020486118
复制
发表时间：
2021-03-30
影响因子：
11.1
通讯作者：
Liu H
中科院分区：
文献类型：
--
作者：
Yun JH;Li X;Yue J;Park JH;Jin Z;Li C;Hu H;Shi Y;Pandey S;Carbajo S;Boutet S;Hunter MS;Liang M;Sierra RG;Lane TJ;Zhou L;Weierstall U;Zatsepin NA;Ohki M;Tame JRH;Park SY;Spence JCH;Zhang W;Schmidt M;Lee W;Liu H
光驱动的视紫红质蛋白质泵送离子穿过细胞膜。它们在光遗传学中有应用，并可能用于开发太阳能收集设备。因此，对视紫红质动力学和功能的详细了解可能有助于医学，健康和清洁能源的研究。用X射线自由电子激光进行的时间分辨晶体学研究揭示了100 ps光激活内氯离子泵浦视紫红质（ClR）的详细动力学。图中显示了光引发的视黄醛异构化作用下，Cl−从席夫碱结合位点上解离。这种Cl−解离之后是向细胞内方向的扩散。结果暗示在一个共同的离子泵机制在视紫红质家族。一些海洋细菌中的氯离子泵视紫红质（ClR）利用光能将Cl−主动运输到细胞中。ClR如何启动传输是难以捉摸的。在这里，我们展示了使用直线加速器相干光源的时间分辨串行飞秒（fs）晶体学观察到的离子输运的动态。X射线脉冲捕获的结构变化，在ClR闪光照明与550 nm飞秒泵浦激光。五个时间点的高分辨率结构（黑暗到100 ps后闪烁）揭示了复杂和协调的动力学，包括视网膜异构化，水分子重排，和各种残基的构象变化。结合时间分辨光谱实验和分子动力学模拟的数据，这项研究表明，氯离子接近希夫碱经历了一个解离扩散过程后，光引发的视网膜异构化。
Light-driven rhodopsin proteins pump ions across cell membranes. They have applications in optogenetics and can potentially be used to develop solar energy–harvesting devices. A detailed understanding of rhodopsin dynamics and functions may therefore assist research in medicine, health, and clean energy. This time-resolved crystallography study carried out with X-ray free-electron lasers reveals detailed dynamics of chloride ion–pumping rhodopsin (ClR) within 100 ps of light activation. It shows the dissociation of Cl− from the Schiff base binding site upon light-triggered retinal isomerization. This Cl− dissociation is followed by diffusion toward the intracellular direction. The results hint at a common ion-pumping mechanism across rhodopsin families. Chloride ion–pumping rhodopsin (ClR) in some marine bacteria utilizes light energy to actively transport Cl− into cells. How the ClR initiates the transport is elusive. Here, we show the dynamics of ion transport observed with time-resolved serial femtosecond (fs) crystallography using the Linac Coherent Light Source. X-ray pulses captured structural changes in ClR upon flash illumination with a 550 nm fs-pumping laser. High-resolution structures for five time points (dark to 100 ps after flashing) reveal complex and coordinated dynamics comprising retinal isomerization, water molecule rearrangement, and conformational changes of various residues. Combining data from time-resolved spectroscopy experiments and molecular dynamics simulations, this study reveals that the chloride ion close to the Schiff base undergoes a dissociation–diffusion process upon light-triggered retinal isomerization.
登录
查看更多内容
DOI：
10.1107/s0907444909029436
发表时间：
2009-10-01
影响因子：
2.2
作者：
Moriarty, Nigel W.;Grosse-Kunstleve, Ralf W.;Adams, Paul D.
通讯作者：
Adams, Paul D.
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：
16.6
作者：
Kim K;Kwon SK;Jun SH;Cha JS;Kim H;Lee W;Kim JF;Cho HS
通讯作者：
Cho HS
影响因子：
5.5
作者：
Best, Robert B.;Zhu, Xiao;Shim, Jihyun;Lopes, Pedro E. M.;Mittal, Jeetain;Feig, Michael;MacKerell, Alexander D., Jr.
通讯作者：
MacKerell, Alexander D., Jr.
DOI：
10.1107/s0907444909052925
发表时间：
2010-02
期刊：
Acta crystallographica. Section D, Biological crystallography
影响因子：
--
作者：
Adams PD;Afonine PV;Bunkóczi G;Chen VB;Davis IW;Echols N;Headd JJ;Hung LW;Kapral GJ;Grosse-Kunstleve RW;McCoy AJ;Moriarty NW;Oeffner R;Read RJ;Richardson DC;Richardson JS;Terwilliger TC;Zwart PH
通讯作者：
Zwart PH