Unfolded-State Dynamics and Structure of Protein L Characterized by Simulation and Experiment.

While several experimental techniques now exist for characterizing protein unfolded states, all-atom simulation of unfolded states has been challenging due to the long time scales and conformational sampling required. We address this problem by using a combination of accelerated calculations on grap...

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Publicado en:Journal of the American Chemical Society Vol. 132; no. 13; pp. 4702 - 4710
Autores principales: Voelz, Vincent A., Singh, Vijay R., Wedemeyer, William J., Lapidus, Lisa J., Pande, Vijay S.
Formato: Artículo
Publicado: American Chemical Society 4/7/2010
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Acceso en línea:Ver este registro en EBSCOhost
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      pub: American Chemical Society
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        10.1021/ja908369h
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        atl: Unfolded-State Dynamics and Structure of Protein L Characterized by Simulation and Experiment.
      aug:
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          Voelz, Vincent A.
          Singh, Vijay R.
          Wedemeyer, William J.
          Lapidus, Lisa J.
          Pande, Vijay S.
        affil:
          Department of Chemistry, Stanford University, Stanford, California 94305
          Department of Physics and Astronomy, Michigan State University, East Lansing, Michigan 48824
          Department of Biochemistry and Molecular Biology, Michigan State University, East Lansing, Michigan 48824
      su:
        Denaturation of proteins
        Molecular dynamics
        Chemical research
        Spectrum analysis
        Simulation methods & models
        Equipment & supplies
      sug:
        subj:
          Denaturation of proteins
          Molecular dynamics
          Chemical research
          Spectrum analysis
          Simulation methods & models
          Equipment & supplies
      ab: While several experimental techniques now exist for characterizing protein unfolded states, all-atom simulation of unfolded states has been challenging due to the long time scales and conformational sampling required. We address this problem by using a combination of accelerated calculations on graphics processor units and distributed computing to simulate tens of thousands of molecular dynamics trajectories each up to -∼10 μs (for a total aggregate simulation time of 127 ms). We used this approach in conjunction with Trp-Cys contact quenching experiments to characterize the unfolded structure and dynamics of protein L. We employed a polymer theory method to make quantitative comparisons between high-temperature simulated and chemically denatured experimental ensembles and find that reaction-limited quenching rates calculated from simulation agree remarkably well with experiment. In both experiment and simulation, we find that unfolded-state intramolecular diffusion rates are very slow compared to highly denatured chains and that a single-residue mutation can significantly alter unfolded-state dynamics and structure. This work suggests a view of the unfolded state in which surprisingly low diffusion rates could limit folding and opens the door for all-atom molecular simulation to be a useful predictive tool for characterizing protein unfolded states along with experiments that directly measure intramolecular diffusion.
      pubtype: Academic Journal
      doctype: Article
      src: R
    language: English
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