Optical control of ultrafast structural dynamics in a fluorescent protein.
Optical control of ultrafast structural dynamics in a fluorescent protein.
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荧光蛋白超快结构动力学的光学控制。
DOI：
10.1038/s41557-023-01275-1
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发表时间：
2023-11
期刊：
影响因子：
21.8
通讯作者：
van Thor, Jasper J.
中科院分区：
文献类型：
--
作者：
Hutchison, Christopher D. M.;Baxter, James M.;Fitzpatrick, Ann;Dorlhiac, Gabriel;Fadini, Alisia;Perrett, Samuel;Maghlaoui, Karim;Lefevre, Salome Bodet;Cordon-Preciado, Violeta;Ferreira, Josie L.;Chukhutsina, Volha U.;Garratt, Douglas;Barnard, Jonathan;Galinis, Gediminas;Glencross, Flo;Morgan, Rhodri M.;Stockton, Sian;Taylor, Ben;Yuan, Letong;Romei, Matthew G.;Lin, Chi-Yun;Marangos, Jon P.;Schmidt, Marius;Chatrchyan, Viktoria;Buckup, Tiago;Morozov, Dmitry;Park, Jaehyun;Park, Sehan;Eom, Intae;Kim, Minseok;Jang, Dogeun;Choi, Hyeongi;Hyun, HyoJung;Park, Gisu;Nango, Eriko;Tanaka, Rie;Owada, Shigeki;Tono, Kensuke;DePonte, Daniel P.;Carbajo, Sergio;Seaberg, Matt;Aquila, Andrew;Boutet, Sebastien;Barty, Anton;Iwata, So;Boxer, Steven G.;Groenhof, Gerrit;van Thor, Jasper J.
荧光蛋白发色团的光异构化反应发生在超快时间尺度上。由飞秒光激发产生的结构动力学具有来自振动和电子过程以及涉及通过圆锥交叉的交叉的反应动力学的贡献。超快结构动力学的产生和发展强烈依赖于光学和分子参数。当使用X射线晶体学作为超快动力学的探针时，所观察到的核运动的起源是未知的。现在，高分辨率的泵浦-探测X射线晶体学揭示了荧光蛋白活性位点中复杂的亚稳态、超快运动和氢键重排。然而，我们表明，所测量的运动是不是光异构化反应的一部分，而是产生于脉冲驱动的相干振动过程中的电子基态。使用双色和双脉冲光激发的相干控制实验强烈地放大了X射线晶体学差异密度，而它完全耗尽光致异构化过程。相干控制机制进行了测试，并确认波包分配。抽运-探测测量通常可以实现反应过程的X射线晶体学的飞秒时间分辨率，但测量的结构动力学是复杂的。使用相干控制技术，我们表明，超快的荧光蛋白质的晶体差异占主导地位的基态振动过程是无关的光异构化反应的生色团。
The photoisomerization reaction of a fluorescent protein chromophore occurs on the ultrafast timescale. The structural dynamics that result from femtosecond optical excitation have contributions from vibrational and electronic processes and from reaction dynamics that involve the crossing through a conical intersection. The creation and progression of the ultrafast structural dynamics strongly depends on optical and molecular parameters. When using X-ray crystallography as a probe of ultrafast dynamics, the origin of the observed nuclear motions is not known. Now, high-resolution pump–probe X-ray crystallography reveals complex sub-ångström, ultrafast motions and hydrogen-bonding rearrangements in the active site of a fluorescent protein. However, we demonstrate that the measured motions are not part of the photoisomerization reaction but instead arise from impulsively driven coherent vibrational processes in the electronic ground state. A coherent-control experiment using a two-colour and two-pulse optical excitation strongly amplifies the X-ray crystallographic difference density, while it fully depletes the photoisomerization process. A coherent control mechanism was tested and confirmed the wave packets assignment. Pump–probe measurements conventionally achieve femtosecond time resolution for X-ray crystallography of reactive processes, but the measured structural dynamics are complex. Using coherent control techniques, we show that the ultrafast crystallographic differences of a fluorescent protein are dominated by ground-state vibrational processes that are unconnected to the photoisomerization reaction of the chromophore.
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打开硬件微秒色散瞬态吸收光谱仪，用于线性光学响应。
DOI：
10.1007/s43630-021-00127-6
发表时间：
2022-01
期刊：
Photochemical & photobiological sciences : Official journal of the European Photochemistry Association and the European Society for Photobiology
影响因子：
--
作者：
Hutchison CDM;Parker S;Chukhutsina V;van Thor JJ
通讯作者：
van Thor JJ
DOI：
10.1107/s2059798316010706
发表时间：
2016-08
期刊：
Acta crystallographica. Section D, Structural biology
影响因子：
--
作者：
Ginn HM;Roedig P;Kuo A;Evans G;Sauter NK;Ernst OP;Meents A;Mueller-Werkmeister H;Miller RJ;Stuart DI
通讯作者：
Stuart DI
DOI：
10.1073/pnas.0409035102
发表时间：
2005-05-17
影响因子：
11.1
作者：
Ihee, H;Rajagopal, S;Moffat, K
通讯作者：
Moffat, K
影响因子：
64.8
作者：
Dickson, RM;Cubitt, AB;Moerner, WE
通讯作者：
Moerner, WE
影响因子：
5.6
作者：
Hutchison CDM;Cordon-Preciado V;Morgan RML;Nakane T;Ferreira J;Dorlhiac G;Sanchez-Gonzalez A;Johnson AS;Fitzpatrick A;Fare C;Marangos JP;Yoon CH;Hunter MS;DePonte DP;Boutet S;Owada S;Tanaka R;Tono K;Iwata S;van Thor JJ
通讯作者：
van Thor JJ