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Dielectric dispersion interpretation of single enzyme dynamic disorder, spectral diffusion, and radiative fluorescence lifetime

Prakash, Meher K. and Marcus, R. A. (2008) Dielectric dispersion interpretation of single enzyme dynamic disorder, spectral diffusion, and radiative fluorescence lifetime. Journal of Physical Chemistry B, 112 (2). pp. 399-404. ISSN 1520-6106. doi:10.1021/jp0758869.

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A formulation based on measurable dielectric dispersion of enzymes is developed to estimate fluctuations in electrostatic interaction energy on time scales as long as milliseconds to seconds at a local site in enzymes. Several single molecule experimental observations occur on this time scale, currently unreachable by real time computational trajectory simulations. We compare the experimental results on the autocorrelation function of the fluctuations of catalysis rate with the calculations using the dielectric dispersion formulation. We also discuss the autocorrelation functions of the fluorescence lifetime and of spectral diffusion. We use a previously derived relation between the observables and the electric field fluctuations and calculate the latter using dielectric dispersion data for the proteins and the Onsager regression hypothesis.

Item Type:Article
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URLURL TypeDescription DOIArticle
Marcus, R. A.0000-0001-6547-1469
Additional Information:© 2008 American Chemical Society. Received: July 25, 2007; In Final Form: August 31, 2007. Published on Web October 23, 2007. It is a pleasure to acknowledge the support of this research by the National Science Foundation and the Office of Naval Research. M.K.P. thanks Professor Jovan Mijovic and Yu Bian for helpful discussions.
Funding AgencyGrant Number
Office of Naval Research (ONR)UNSPECIFIED
Issue or Number:2
Record Number:CaltechAUTHORS:20150316-153424442
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Official Citation:Dielectric Dispersion Interpretation of Single Enzyme Dynamic Disorder, Spectral Diffusion, and Radiative Fluorescence Lifetime Meher K. Prakash and and R. A. Marcus The Journal of Physical Chemistry B 2008 112 (2), 399-404 DOI: 10.1021/jp0758869
Usage Policy:No commercial reproduction, distribution, display or performance rights in this work are provided.
ID Code:55819
Deposited By: Tony Diaz
Deposited On:16 Mar 2015 22:43
Last Modified:10 Nov 2021 20:50

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