Second harmonic correlation spectroscopy: a method for determining surface binding kinetics and thermodynamics.
Second harmonic correlation spectroscopy: a method for determining surface binding kinetics and thermodynamics.
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二次谐波相关光谱：一种确定表面结合动力学和热力学的方法。
DOI：
10.1021/ac4018742
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发表时间：
2013
影响因子：
7.4
通讯作者：
Conboy,JohnC
中科院分区：
文献类型：
--
作者：
Sly,KrystalL;Mok,Sze-Wing;Conboy,JohnC
这些研究描述了实施二次谐波相关光谱（SHCS）来测量与表面相关的分子物种的吸附和解吸动力学。具体地说，利用二次谐波信号的局域涨落来确定（S）-（+）-1，1 ′-联-2-萘SBN嵌入1，2-二油酰基-sn-甘油基-3-磷酸胆碱（DOPC）双层的结合动力学和热力学.为了确定吸附和解吸速率，在稳态平衡下高于饱和浓度时收集SH信号作为时间的函数。然后将自相关SH信号拟合到针对当溶液中的分子没有贡献时在表面处结合的分子开发的相关模型。SBN在DOPC上的吸附速率为2.7 ± 0.2 × 10 ~（-3）s ~（-1）M ~（-1），解吸速率为9 ± 4 × 10 ~（-4）s ~（-1）。由SHCS法求得的动力学速率和平衡结合常数（3.0 ± 1.3 × 106 M ~（-1））与由传统结合等温线法求得的结果进行了比较，发现两者在统计学上是一致的。使用SHCS的主要优点是在同一实验中仅使用单一本体浓度的SBN来测定吸收和解吸速率。这些研究的结果表明，SHCS可用于提供准确的动力学和热力学结合数据，在一个无标记的方式代替传统的等温线研究，特别是在时间和分析物是稀缺的。
These studies describe the implementation of second harmonic correlation spectroscopy (SHCS) to measure the adsorption and desorption kinetics of molecular species associated with a surface. Specifically, the local fluctuations of the measured second harmonic (SH) signal were used to determine the binding kinetics and thermodynamics of (S)-(+)-1,1′-bi-2-napthol SBN intercalation into a 1,2-dioleoyl-sn-glycero-3-phosphocoline (DOPC) bilayer. In order to determine the adsorption and desorption rates, the SH signal was collected above saturation concentration at steady-state equilibrium as a function of time. The autocorrelated SH signal was then fit to a correlation model developed for molecules binding at a surface when there is no contribution from molecules in solution. The measured adsorption rate for SBN to DOPC was 2.7 ± 0.2 × 103s–1M–1and the desorption rate was 9 ± 4 × 10–4s–1. The kinetic rates as well as the calculated equilibrium binding constant, 3.0 ± 1.3 × 106M–1obtained from SHCS were compared with those obtained from a conventional binding isotherm and found to be statistically consistent. The primary advantage of using SHCS is both the absorption and desorption rates were determined in the same experiment using only a single bulk concentration of SBN. The results of these studies demonstrate that SHCS can be used to provide accurate kinetic and thermodynamic binding data in a label-free manner in lieu of conventional isotherm studies, especially where time and analyte are scarce.