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首页> 外文期刊>The journal of physical chemistry, A. Molecules, spectroscopy, kinetics, environment, & general theory >Femtosecond Heterodyne-Detected Four-Wave-Mixing Studies of Deterministic Protein Motions. 1. Theory and Experimental Technique of Diffractive Optics-Based Spectroscopy
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Femtosecond Heterodyne-Detected Four-Wave-Mixing Studies of Deterministic Protein Motions. 1. Theory and Experimental Technique of Diffractive Optics-Based Spectroscopy

机译：飞秒外差检测的确定性蛋白运动的四波混频研究。 1.基于衍射光学光谱的理论和实验技术

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摘要

Analytic relations are developed to describe the coupling between experimentally observed optically heterodyne-detected (OHD) transient grating (TG) signals and the underlying molecular dynamics of heme proteins. The heterodyne detection was implemented using a diffractive optical element to generate the phase-matched beam pattern along with a reference beam for OHD. The phase stability between the reference and signal fields using this approach is shown to be excellent over several hours of signal collection. Under small signal conditions this leads to an enhancement in signal-to-noise of several orders of magnitude. The grating excitation provides an inherent acoustic reference that can be used to determine the absolute signal phase. This enables separation of the real and imaginary components to the nonlinear susceptibility as well as determination of both the absorption anisotropy and its real counterpart, the phase anisotropy. The relationship between the phase anisotropy and the observed OHD TG signals is expressed in terms of the complex molecular polarizability specific to heme proteins but can be readily extended to all other systems. Access to the material anisotropy provides a direct probe of mode selective coupling in proteins, i.e., the nonuniform displacements determined by the underlying asymmetric protein structure.
机译：建立了解析关系，以描述实验观察到的光学外差检测（OHD）瞬态光栅（TG）信号与血红素蛋白潜在的分子动力学之间的耦合。外差检测是使用衍射光学元件实现的，以生成相位匹配的光束方向图以及用于OHD的参考光束。使用这种方法，参考场和信号场之间的相位稳定性在信号采集的几个小时内表现出了出色的表现。在小信号条件下，这会导致信噪比提高几个数量级。光栅激励提供了固有的声学参考，可用于确定绝对信号相位。这使得能够将实部和虚部分离为非线性磁化率，并确定吸收各向异性及其真实对应物（即相位各向异性）。相异性和观察到的OHD TG信号之间的关系以血红素蛋白特有的复杂分子极化率表示，但可以很容易地扩展到所有其他系统。接近材料各向异性提供了蛋白质中模式选择性偶联的直接探针，即由下面的不对称蛋白质结构决定的不均匀位移。

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