An ultrasensitive tool exploiting hydration dynamics to decipher weak lipid membrane-polymer interactions

Chi Yuan Cheng; Jia Yu Wang; Ravinath Kausik; Ka Yee C. Lee; Songi Han

doi:10.1016/j.jmr.2011.12.004

An ultrasensitive tool exploiting hydration dynamics to decipher weak lipid membrane-polymer interactions

Chi Yuan Cheng, Jia Yu Wang, Ravinath Kausik, Ka Yee C. Lee^*, Songi Han

^*Corresponding author for this work

Chemistry

Research output: Contribution to journal › Article › peer-review

30 Scopus citations

Abstract

We introduce a newly developed tool, ¹H Overhauser Dynamic Nuclear Polarization (ODNP), to sensitively explore weak macromolecular interactions by site-specifically probing the modulation of the translational dynamics of hydration water at the interaction interface, in the full presence of bulk water. Here, ODNP is employed on an illustrative example of a membrane-active triblock copolymer, poloxamer 188 (P188), which is known to restore the integrity of structurally compromised cell membranes. We observe a distinct change in the translational dynamics of the hydration layer interacting with the lipid membrane surface and the bilayer-interior as P188 is added to a solution of lipid vesicles, but no measurable changes in the dynamics or structure of the lipid membranes. This study shows that hydration water is an integral constituent of a lipid membrane system, and demonstrates for the first time that the modulation of its translational diffusivity can sensitively report on weak polymer-membrane interactions, as well as mediate essential lipid membrane functions. ODNP holds much promise as a unique tool to unravel molecular interactions at interfaces even in the presence of bulk water under ambient conditions.

Original language	English (US)
Pages (from-to)	115-119
Number of pages	5
Journal	Journal of Magnetic Resonance
Volume	215
DOIs	https://doi.org/10.1016/j.jmr.2011.12.004
State	Published - Feb 2011

Funding

C.-Y.C., R.K., and S.H. acknowledge for the support of the UCSB NSF-MRSEC Program (DMR05-20415), the NSF Faculty Early CAREER Award (CHE-0645536) and the Packard Fellowship for Science and Engineering. J.-Y.W. and K.Y.C.L. are grateful for the support of the March of Dimes (No. 6-FY07-357), the NSF (MCB-0920316) and the University of Chicago NSF-MRSEC program (DMR-0820054).

Keywords

Dynamic nuclear polarization
Hydration dynamics
Hyperpolarization
Overhauser effect
Polymer-lipid interaction

ASJC Scopus subject areas

Condensed Matter Physics
Nuclear and High Energy Physics
Biophysics
Biochemistry

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10.1016/j.jmr.2011.12.004

Cite this

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title = "An ultrasensitive tool exploiting hydration dynamics to decipher weak lipid membrane-polymer interactions",

abstract = "We introduce a newly developed tool, 1H Overhauser Dynamic Nuclear Polarization (ODNP), to sensitively explore weak macromolecular interactions by site-specifically probing the modulation of the translational dynamics of hydration water at the interaction interface, in the full presence of bulk water. Here, ODNP is employed on an illustrative example of a membrane-active triblock copolymer, poloxamer 188 (P188), which is known to restore the integrity of structurally compromised cell membranes. We observe a distinct change in the translational dynamics of the hydration layer interacting with the lipid membrane surface and the bilayer-interior as P188 is added to a solution of lipid vesicles, but no measurable changes in the dynamics or structure of the lipid membranes. This study shows that hydration water is an integral constituent of a lipid membrane system, and demonstrates for the first time that the modulation of its translational diffusivity can sensitively report on weak polymer-membrane interactions, as well as mediate essential lipid membrane functions. ODNP holds much promise as a unique tool to unravel molecular interactions at interfaces even in the presence of bulk water under ambient conditions.",

keywords = "Dynamic nuclear polarization, Hydration dynamics, Hyperpolarization, Overhauser effect, Polymer-lipid interaction",

author = "Cheng, \{Chi Yuan\} and Wang, \{Jia Yu\} and Ravinath Kausik and Lee, \{Ka Yee C.\} and Songi Han",

note = "Funding Information: C.-Y.C., R.K., and S.H. acknowledge for the support of the UCSB NSF-MRSEC Program (DMR05-20415), the NSF Faculty Early CAREER Award (CHE-0645536) and the Packard Fellowship for Science and Engineering. J.-Y.W. and K.Y.C.L. are grateful for the support of the March of Dimes (No. 6-FY07-357), the NSF (MCB-0920316) and the University of Chicago NSF-MRSEC program (DMR-0820054). ",

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AU - Cheng, Chi Yuan

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AU - Kausik, Ravinath

AU - Lee, Ka Yee C.

AU - Han, Songi

N1 - Funding Information: C.-Y.C., R.K., and S.H. acknowledge for the support of the UCSB NSF-MRSEC Program (DMR05-20415), the NSF Faculty Early CAREER Award (CHE-0645536) and the Packard Fellowship for Science and Engineering. J.-Y.W. and K.Y.C.L. are grateful for the support of the March of Dimes (No. 6-FY07-357), the NSF (MCB-0920316) and the University of Chicago NSF-MRSEC program (DMR-0820054).

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N2 - We introduce a newly developed tool, 1H Overhauser Dynamic Nuclear Polarization (ODNP), to sensitively explore weak macromolecular interactions by site-specifically probing the modulation of the translational dynamics of hydration water at the interaction interface, in the full presence of bulk water. Here, ODNP is employed on an illustrative example of a membrane-active triblock copolymer, poloxamer 188 (P188), which is known to restore the integrity of structurally compromised cell membranes. We observe a distinct change in the translational dynamics of the hydration layer interacting with the lipid membrane surface and the bilayer-interior as P188 is added to a solution of lipid vesicles, but no measurable changes in the dynamics or structure of the lipid membranes. This study shows that hydration water is an integral constituent of a lipid membrane system, and demonstrates for the first time that the modulation of its translational diffusivity can sensitively report on weak polymer-membrane interactions, as well as mediate essential lipid membrane functions. ODNP holds much promise as a unique tool to unravel molecular interactions at interfaces even in the presence of bulk water under ambient conditions.

AB - We introduce a newly developed tool, 1H Overhauser Dynamic Nuclear Polarization (ODNP), to sensitively explore weak macromolecular interactions by site-specifically probing the modulation of the translational dynamics of hydration water at the interaction interface, in the full presence of bulk water. Here, ODNP is employed on an illustrative example of a membrane-active triblock copolymer, poloxamer 188 (P188), which is known to restore the integrity of structurally compromised cell membranes. We observe a distinct change in the translational dynamics of the hydration layer interacting with the lipid membrane surface and the bilayer-interior as P188 is added to a solution of lipid vesicles, but no measurable changes in the dynamics or structure of the lipid membranes. This study shows that hydration water is an integral constituent of a lipid membrane system, and demonstrates for the first time that the modulation of its translational diffusivity can sensitively report on weak polymer-membrane interactions, as well as mediate essential lipid membrane functions. ODNP holds much promise as a unique tool to unravel molecular interactions at interfaces even in the presence of bulk water under ambient conditions.

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KW - Hydration dynamics

KW - Hyperpolarization

KW - Overhauser effect

KW - Polymer-lipid interaction

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ER -

An ultrasensitive tool exploiting hydration dynamics to decipher weak lipid membrane-polymer interactions

Abstract

Funding

Keywords

ASJC Scopus subject areas

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