化学
分子动力学
固态核磁共振
磁偶极-偶极相互作用
化学物理
分子
核磁共振波谱
膜
生物分子
胆固醇
动力学(音乐)
生物物理学
偶极子
计算化学
核磁共振
立体化学
生物化学
物理
生物
有机化学
声学
作者
Lisa A. Della Ripa,Joseph M. Courtney,Samantha M Phinney,Collin G. Borcik,Martin D. Burke,Chad M. Rienstra,Taras V. Pogorelov
摘要
Cholesterol promotes the structural integrity of the fluid cell membrane and interacts dynamically with many membrane proteins to regulate function. Understanding site-resolved cholesterol structural dynamics is thus important. This long-standing challenge has thus far been addressed, in part, by selective isotopic labeling approaches. Here we present a new 3D solid-state NMR (SSNMR) experiment utilizing scalar 13C-13C polarization transfer and recoupling of the 1H-13C interactions in order to determine average dipolar couplings for all 1H-13C vectors in uniformly 13C-enriched cholesterol. The experimentally determined order parameters (OP) agree exceptionally well with molecular dynamics (MD) trajectories and reveal coupling among several conformational degrees of freedom in cholesterol molecules. Quantum chemistry shielding calculations further support this conclusion and specifically demonstrate that ring tilt and rotation are coupled to changes in tail conformation and that these coupled segmental dynamics dictate the orientation of cholesterol. These findings advance our understanding of physiologically relevant dynamics of cholesterol, and the methods that revealed them have broader potential to characterize how structural dynamics of other small molecules impact their biological functions.
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