Sum frequency generation and solid-state NMR study of the structure, orientation, and dynamics of polystyrene-adsorbed peptides

被引:128
作者
Weidner, Tobias [1 ,2 ]
Breen, Nicholas F. [3 ]
Li, Kun [3 ,4 ]
Drobny, Gary P. [3 ,4 ]
Castner, David G. [1 ,2 ,5 ]
机构
[1] Univ Washington, Dept Bioengn, Seattle, WA 98195 USA
[2] Univ Washington, Natl ESCA & Surface Anal Ctr Biomed Problems, Seattle, WA 98195 USA
[3] Univ Washington, Dept Chem, Seattle, WA 98195 USA
[4] Univ Washington, Dept Phys, Seattle, WA 98195 USA
[5] Univ Washington, Dept Chem Engn, Seattle, WA 98195 USA
基金
美国国家卫生研究院;
关键词
protein; surface; isotope labels; solid-liquid interface; SIDE-CHAIN; IN-SITU; VIBRATIONAL SPECTROSCOPY; HYDROPHOBIC POLYSTYRENE; MAGNETIC-RESONANCE; HYDROPHILIC SILICA; MODEL PEPTIDES; ADSORPTION; INTERFACES; STATHERIN;
D O I
10.1073/pnas.1003832107
中图分类号
O [数理科学和化学]; P [天文学、地球科学]; Q [生物科学]; N [自然科学总论];
学科分类号
07 ; 0710 ; 09 ;
摘要
The power of combining sum frequency generation (SFG) vibrational spectroscopy and solid-state nuclear magnetic resonance (ssNMR) spectroscopy to quantify, with site specificity and atomic resolution, the orientation and dynamics of side chains in synthetic model peptides adsorbed onto polystyrene (PS) surfaces is demonstrated in this study. Although isotopic labeling has long been used in ssNMR studies to site-specifically probe the structure and dynamics of biomolecules, the potential of SFG to probe side chain orientation in isotopically labeled surface-adsorbed peptides and proteins remains largely unexplored. The 14 amino acid leucine-lysine peptide studied in this work is known to form an a-helical secondary structure at liquid-solid interfaces. Selective, individual deuteration of the isopropyl group in each leucine residue was used to probe the orientation and dynamics of each individual leucine side chain of LK alpha 14 adsorbed onto PS. The selective isotopic labeling methods allowed SFG analysis to determine the orientations of individual side chains in adsorbed peptides. Side chain dynamics were obtained by fitting the deuterium ssNMR line shape to specific motional models. Through the combined use of SFG and ssNMR, the dynamic trends observed for individual side chains by ssNMR have been correlated with side chain orientation relative to the PS surface as determined by SFG. This combination provides a more complete and quantitative picture of the structure, orientation, and dynamics of these surface-adsorbed peptides than could be obtained if either technique were used separately.
引用
收藏
页码:13288 / 13293
页数:6
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