Picosecond dynamics of a membrane protein revealed by 2D IR

Proceedings of the National Academy of Sciences of the United States of America
Prabuddha MukherjeeMartin T Zanni

Abstract

Fast protein dynamics can be missed with techniques that have relatively slow observation times. Using 2D IR spectroscopy and isotope labeling, we have probed the rapid, picosecond dynamics of a membrane protein in its native environment. By measuring the homogeneous and inhomogeneous IR linewidths of 11 amide I modes (backbone carbonyl stretch), we have captured the structural distributions and dynamics of the CD3zeta protein along its transmembrane segment that are lost with slower time-scale techniques. We find that the homogeneous lifetimes and population relaxation times are the same for almost all of the residues. In contrast, the inhomogeneous linewidths vary significantly with the largest inhomogeneous distribution occurring for residues near the N terminus and the narrowest near the center. This behavior is highly consistent with a recently reported experimental model of the protein and water accessibility as observed by molecular dynamics simulations. The data support the proposed CD3zeta peptide structure, and the simulations point to the structural disorder of water and lipid head-groups as the main source of inhomogeneous broadening. Taken together, this rigorous analysis of the vibrational dynamics of a membrane p...Continue Reading

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Citations

Sep 16, 2011·Journal of the American Chemical Society·Lu WangJames L Skinner
Dec 1, 2006·The Journal of Physical Chemistry. B·Prabuddha MukherjeeMartin T Zanni
Dec 15, 2007·The Journal of Physical Chemistry. B·Jianping WangRobin Hochstrasser
Mar 25, 2011·The Journal of Physical Chemistry. a·William J GloverBenjamin J Schwartz
Mar 17, 2011·The Journal of Physical Chemistry. B·L WangJ L Skinner
Mar 16, 2012·The Journal of Physical Chemistry. B·Sayan BagchiMichael D Fayer
Aug 3, 2012·The Journal of Physical Chemistry. B·Lu Wang, James L Skinner
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Jul 24, 2008·The Journal of Physical Chemistry. B·Seongheun KimM D Fayer
Apr 9, 2009·The Journal of Physical Chemistry. B·Yung Sam Kim, Robin M Hochstrasser
Apr 7, 2009·Proceedings of the National Academy of Sciences of the United States of America·Sang-Hee ShimMartin T Zanni
Oct 10, 2009·Proceedings of the National Academy of Sciences of the United States of America·Yung Sam KimRobin M Hochstrasser
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