Ultrafast energy transfer between lipid-linked chromophores and plant light-harvesting complex II.
Ultrafast energy transfer between lipid-linked chromophores and plant light-harvesting complex II.
复制标题
DOI：
10.1039/d1cp01628h
复制
发表时间：
2021-09-15
期刊：
影响因子：
--
通讯作者：
Adams PG
中科院分区：
文献类型：
--
作者：
Hancock AM;Son M;Nairat M;Wei T;Jeuken LJC;Duffy CDP;Schlau-Cohen GS;Adams PG
捕光复合体II(LHCII)是植物叶绿体中发现的一种膜蛋白，它具有吸收太阳能并将激发能量传递给光系统II反应中心亚单位的关键作用。LHCII对蓝光和红光有很强的吸收，但在太阳辐射最大的绿色光谱区域吸收最少。在最近的一项原理证明研究中，我们通过开发一种生物杂交系统来增强这一光谱范围内的吸收，其中LHCII蛋白与脂质连接的德克萨斯红(TR)发色团组装成脂质膜小泡。由于蛋白质-蛋白质相互作用和异质脂结构，这些系统的应用受到了显著的LHCII猝灭的限制。在这里，我们将tr和LHCII组织成一个脂质纳米盘，它提供了一个均匀的、可控的平台来研究tr分子和单个LHCII络合物之间的相互作用。荧光光谱分析表明，tr-to-LHCII的能量转移效率至少为60%，导致LHCII在525-625 nm范围内的荧光增强了262%，是以前系统的两倍。超快瞬时吸收光谱显示了从tR到LHCII能量转移的两个时间常数分别为3.7和128ps。结构建模和理论计算表明，这些时间尺度分别对应于与蛋白质松散或紧密相关的tr-脂，估计tr到LHCII的分离为∼3.5nM和∼1 nm。总之，我们证明了基于纳米盘的生物杂化系统为探索外在发色团和膜蛋白之间的光物理相互作用提供了一个理想的平台，在理解更复杂的自然或人工光合作用系统方面具有潜在的应用前景。我们利用光学光谱、模拟和理论模型表征了脂质连接的发色团和纳米盘中的植物捕光蛋白之间的光物理相互作用。
Light-Harvesting Complex II (LHCII) is a membrane protein found in plant chloroplasts that has the crucial role of absorbing solar energy and subsequently performing excitation energy transfer to the reaction centre subunits of Photosystem II. LHCII provides strong absorption of blue and red light, however, it has minimal absorption in the green spectral region where solar irradiance is maximal. In a recent proof-of-principle study, we enhanced the absorption in this spectral range by developing a biohybrid system where LHCII proteins together with lipid-linked Texas Red (TR) chromophores were assembled into lipid membrane vesicles. The utility of these systems was limited by significant LHCII quenching due to protein–protein interactions and heterogeneous lipid structures. Here, we organise TR and LHCII into a lipid nanodisc, which provides a homogeneous, well-controlled platform to study the interactions between TR molecules and single LHCII complexes. Fluorescence spectroscopy determined that TR-to-LHCII energy transfer has an efficiency of at least 60%, resulting in a 262% enhancement of LHCII fluorescence in the 525–625 nm range, two-fold greater than in the previous system. Ultrafast transient absorption spectroscopy revealed two time constants of 3.7 and 128 ps for TR-to-LHCII energy transfer. Structural modelling and theoretical calculations indicate that these timescales correspond to TR–lipids that are loosely- or tightly-associated with the protein, respectively, with estimated TR-to-LHCII separations of ∼3.5 nm and ∼1 nm. Overall, we demonstrate that a nanodisc-based biohybrid system provides an idealised platform to explore the photophysical interactions between extrinsic chromophores and membrane proteins with potential applications in understanding more complex natural or artificial photosynthetic systems. We characterize the photophysical interactions between lipid-linked chromophores and plant light-harvesting proteins incorporated into nanodiscs using optical spectroscopy, simulations and theoretical modelling.
登录
查看更多内容
DOI：
10.1016/j.bbabio.2018.06.011
发表时间：
2018-10
期刊：
Biochimica et biophysica acta. Bioenergetics
影响因子：
--
作者：
Adams PG;Vasilev C;Hunter CN;Johnson MP
通讯作者：
Johnson MP
影响因子：
16.6
作者：
Grayson KJ;Faries KM;Huang X;Qian P;Dilbeck P;Martin EC;Hitchcock A;Vasilev C;Yuen JM;Niedzwiedzki DM;Leggett GJ;Holten D;Kirmaier C;Neil Hunter C
通讯作者：
Neil Hunter C
影响因子：
3.9
作者：
Gupta, Gautam;Rathod, Shailendra B.;Lopez, Gabriel P.
通讯作者：
Lopez, Gabriel P.
影响因子：
4.6
作者：
Akhunzada, Muhammad Jan;D'Autilia, Francesca;Brancato, Giuseppe
通讯作者：
Brancato, Giuseppe
影响因子：
15
作者：
Bennett, Doran I. G.;Amarnath, Kapil;Fleming, Graham R.
通讯作者：
Fleming, Graham R.