DOI: 10.1073/pnas.0408646102. Conformational changes during the nanosecond-to-millisecond unfolding of ubiquitin

Conformational changes during the nanosecond-to-millisecond unfolding of ubiquitin

10.1073/pnas.0408646102

Crossref journal-article

Proceedings of the National Academy of Sciences

Proceedings of the National Academy of Sciences (341)

Abstract

Steady-state and transient conformational changes upon the thermal unfolding of ubiquitin were investigated with nonlinear IR spectroscopy of the amide I vibrations. Equilibrium temperature-dependent 2D IR spectroscopy reveals the unfolding of the β-sheet of ubiquitin through the loss of cross peaks formed between transitions arising from delocalized vibrations of the β-sheet. Transient unfolding after a nanosecond temperature jump is monitored with dispersed vibrational echo spectroscopy, a projection of the 2D IR spectrum. Whereas the equilibrium study follows a simple two-state unfolding, the transient experiments observe complex relaxation behavior that differs for various spectral components and spans 6 decades in time. The transient behavior can be separated into fast and slow time scales. From 100 ns to 0.5 ms, the spectral features associated with β-sheet unfolding relax in a sequential, nonexponential manner, with time constants of 3 μs and 80 μs. By modeling the amide I vibrations of ubiquitin, this observation is explained as unfolding of the less stable strands III–V of the β-sheet before unfolding of the hairpin that forms part of the hydrophobic core. This downhill unfolding is followed by exponential barrier-crossing kinetics on a 3-ms time scale.

Bibliography

Chung, H. S., Khalil, M., Smith, A. W., Ganim, Z., & Tokmakoff, A. (2005). Conformational changes during the nanosecond-to-millisecond unfolding of ubiquitin. Proceedings of the National Academy of Sciences, 102(3), 612â617.

Authors 5

Hoi Sung Chung (first)
Munira Khalil (additional)
Adam W. Smith (additional)
Ziad Ganim (additional)
Andrei Tokmakoff (additional)

References 49 Referenced 145

Dates

Type	When
Created	20 years, 7 months ago (Jan. 3, 2005, 8:15 p.m.)
Deposited	3 years, 4 months ago (April 25, 2022, 11:02 p.m.)
Indexed	1 year ago (Aug. 26, 2024, 4:26 a.m.)
Issued	20 years, 7 months ago (Jan. 3, 2005)
Published	20 years, 7 months ago (Jan. 3, 2005)
Published Online	20 years, 7 months ago (Jan. 3, 2005)
Published Print	20 years, 7 months ago (Jan. 18, 2005)

Funders 0

None

BibTeX

@article{Chung_2005, title={Conformational changes during the nanosecond-to-millisecond unfolding of ubiquitin}, volume={102}, ISSN={1091-6490}, url={http://dx.doi.org/10.1073/pnas.0408646102}, DOI={10.1073/pnas.0408646102}, number={3}, journal={Proceedings of the National Academy of Sciences}, publisher={Proceedings of the National Academy of Sciences}, author={Chung, Hoi Sung and Khalil, Munira and Smith, Adam W. and Ganim, Ziad and Tokmakoff, Andrei}, year={2005}, month=jan, pages={612–617} }

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  "abstract": "<jats:p>Steady-state and transient conformational changes upon the thermal unfolding of ubiquitin were investigated with nonlinear IR spectroscopy of the amide I vibrations. Equilibrium temperature-dependent 2D IR spectroscopy reveals the unfolding of the \u03b2-sheet of ubiquitin through the loss of cross peaks formed between transitions arising from delocalized vibrations of the \u03b2-sheet. Transient unfolding after a nanosecond temperature jump is monitored with dispersed vibrational echo spectroscopy, a projection of the 2D IR spectrum. Whereas the equilibrium study follows a simple two-state unfolding, the transient experiments observe complex relaxation behavior that differs for various spectral components and spans 6 decades in time. The transient behavior can be separated into fast and slow time scales. From 100 ns to 0.5 ms, the spectral features associated with \u03b2-sheet unfolding relax in a sequential, nonexponential manner, with time constants of 3 \u03bcs and 80 \u03bcs. By modeling the amide I vibrations of ubiquitin, this observation is explained as unfolding of the less stable strands III\u2013V of the \u03b2-sheet before unfolding of the hairpin that forms part of the hydrophobic core. This downhill unfolding is followed by exponential barrier-crossing kinetics on a 3-ms time scale.</jats:p>",
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