Complexation of Green and Red Kaede Fluorescent Protein Chromophores by a Zwitterion to Probe Electrostatic and Induction Field Effects.
Complexation of Green and Red Kaede Fluorescent Protein Chromophores by a Zwitterion to Probe Electrostatic and Induction Field Effects.
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绿色和红色Kaede荧光蛋白发色团的络合通过s扭转，以探测静电和诱导场效应。
DOI：
10.1021/acs.jpca.1c10628
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发表时间：
2022-02-24
影响因子：
2.9
通讯作者：
Bull, James N.
中科院分区：
文献类型：
--
作者：
Ashworth, Eleanor K.;Stockett, Mark H.;Kjaer, Christina;Page, Philip C. Bulman;Meech, Stephen R.;Nielsen, Steen Brondsted;Bull, James N.
绿色荧光蛋白(GFP)和红色凯德荧光蛋白(RKFP)的光物理是由光吸收发色团的固有性质及其与蛋白质结合口袋的相互作用决定的。这项工作利用光解离作用光谱探测了一系列合成的GFP和rKFP生色团作为裸阴离子和甜菜碱两性离子络合物的吸收曲线，这被认为是偶极微溶剂化的模型。采用对称性适应微扰理论的电子结构计算和能量分解分析来表征气相结构和复杂的内聚力。计算表明甜菜碱与苯氧基去质子化中心的配位优势主要是通过静电力。用STEOM-DLPNO-CCSD方法计算得到了裸阴离子和阴离子-甜菜碱络合物的绝对和相对垂直激发能。另一方面，用点电荷模型处理甜菜碱分子，其中电荷是根据一些常见的电子密度布居分析方案计算的，结果表明，只有静电和点电荷诱导相互作用不能解释甜菜碱诱导的光谱移动。本方法也可用于研究其他气相离子-两性离子络合物的团簇力和光学性质。
The photophysics of green fluorescent protein (GFP) and red Kaede fluorescent protein (rKFP) are defined by the intrinsic properties of the light-absorbing chromophore and its interaction with the protein binding pocket. This work deploys photodissociation action spectroscopy to probe the absorption profiles for a series of synthetic GFP and rKFP chromophores as the bare anions and as complexes with the betaine zwitterion, which is assumed as a model for dipole microsolvation. Electronic structure calculations and energy decomposition analysis using Symmetry-Adapted Perturbation Theory are used to characterize gas-phase structures and complex cohesion forces. The calculations reveal a preponderance for coordination of betaine to the phenoxide deprotonation site predominantly through electrostatic forces. Calculations using the STEOM-DLPNO-CCSD method are able to reproduce absolute and relative vertical excitation energies for the bare anions and anion–betaine complexes. On the other hand, treatment of the betaine molecule with a point-charge model, in which the charges are computed from some common electron density population analysis schemes, show that just electrostatic and point-charge induction interactions are unable to account for the betaine-induced spectral shift. The present methodology could be applied to investigate cluster forces and optical properties in other gas-phase ion–zwitterion complexes.
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影响因子：
4.4
作者：
Hohenstein, Edward G.;Sherrill, C. David
通讯作者：
Sherrill, C. David
影响因子：
5.5
作者：
Filippi, Claudia;Buda, Francesco;Sinicropi, Adalgisa
通讯作者：
Sinicropi, Adalgisa
影响因子：
5.7
作者：
Loos, Pierre-Francois;Scemama, Anthony;Jacquemin, Denis
通讯作者：
Jacquemin, Denis
影响因子：
2.9
作者：
Bull, James N.;da Silva, Gabriel;Bieske, Evan J.
通讯作者：
Bieske, Evan J.
影响因子：
1.8
作者：
Forbes, Matthew W.;Nagy, Andrea M.;Jockusch, Rebecca A.
通讯作者：
Jockusch, Rebecca A.