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Segmental Dynamics of Membranous Cholesterol are Coupled

  • Lisa A. Della Ripa
    Lisa A. Della Ripa
    Department of Chemistry, University of Illinois at Urbana─Champaign, Urbana, Illinois 61801, United States
  • Joseph M. Courtney
    Joseph M. Courtney
    Department of Chemistry, University of Illinois at Urbana─Champaign, Urbana, Illinois 61801, United States
  • Samantha M. Phinney
    Samantha M. Phinney
    Department of Biochemistry, University of Illinois at Urbana─Champaign, Urbana, Illinois 61801, United States
  • Collin G. Borcik
    Collin G. Borcik
    Department of Biochemistry, University of Wisconsin─Madison, Madison, Wisconsin 53706, United States
  • Martin D. Burke*
    Martin D. Burke
    Department of Chemistry,  Department of Biochemistry,  Beckman Institute for Advanced Science and Technology  and  Carle Illinois College of Medicine, University of Illinois at Urbana─Champaign, Urbana, Illinois 61801, United States
    *[email protected]
  • Chad M. Rienstra*
    Chad M. Rienstra
    Department of Biochemistry,  National Magnetic Resonance Facility at Madison  and  Morgridge Institute for Research, University of Wisconsin─Madison, Madison, Wisconsin 53706, United States
    *[email protected]
  • , and 
  • Taras V. Pogorelov*
    Taras V. Pogorelov
    Department of Chemistry,  Center for Biophysics and Quantitative Biology,  School of Chemical Sciences,  National Center for Supercomputing Applications  and  Beckman Institute for Advanced Science and Technology, University of Illinois at Urbana─Champaign, Urbana, Illinois 61801, United States
    *[email protected]
Cite this: J. Am. Chem. Soc. 2023, 145, 28, 15043–15048
Publication Date (Web):July 6, 2023
https://doi.org/10.1021/jacs.3c01775
Copyright © 2023 American Chemical Society

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    Abstract

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    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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