Numerical Simulation of Vibrational Sum Frequency Generation Intensity for Non-Centrosymmetric Domains Interspersed in an Amorphous Matrix: A Case Study for Cellulose in Plant Cell Wall,The Journal of Physical Chemistry B

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Numerical Simulation of Vibrational Sum Frequency Generation Intensity for Non-Centrosymmetric Domains Interspersed in an Amorphous Matrix: A Case Study for Cellulose in Plant Cell Wall
The Journal of Physical Chemistry B ( IF 2.8 ) Pub Date : 2022-08-29 , DOI: 10.1021/acs.jpcb.2c03897
Juseok Choi ₁ , Jongcheol Lee ₁ , Mohamadamin Makarem ₁ , Shixin Huang ₁ , Seong H Kim ₁

Affiliation

Vibrational sum frequency generation (SFG) spectroscopy can specifically probe molecular species non-centrosymmetrically arranged in a centrosymmetric or isotropic medium. This capability has been extensively utilized to detect and study molecular species present at the two-dimensional (2D) interface at which the centrosymmetry or isotropy of bulk phases is naturally broken. The same principle has been demonstrated to be very effective for the selective detection of non-centrosymmetric crystalline nanodomains interspersed in three-dimensional (3D) amorphous phases. However, the full spectral interpretation of SFG features has been difficult due to the complexity associated with the theoretical calculation of SFG responses of such 3D systems. This paper describes a numerical method to predict the relative SFG intensities of non-centrosymmetric nanodomains in 3D systems as functions of their size and concentration as well as their assembly patterns, i.e., the distributions of tilt, azimuth, and rotation angles with respect to the lab coordinate. We applied the developed method to predict changes in the CH and OH stretch modes characteristic to crystalline cellulose microfibrils distributed with various orders, which are relevant to plant cell wall structures. The same algorithm can also be applied to any SFG-active nanodomains interspersed in 3D amorphous matrices.

中文翻译：

散布在无定形基质中的非中心对称域的振动和频产生强度的数值模拟：植物细胞壁中纤维素的案例研究

振动和频产生 (SFG) 光谱可以专门探测在中心对称或各向同性介质中非中心对称排列的分子种类。这种能力已被广泛用于检测和研究存在于二维 (2D) 界面上的分子种类，在该界面处，体相的中心对称性或各向同性自然被破坏。已证明相同原理对于选择性检测散布在三维 (3D) 非晶相中的非中心对称结晶纳米域非常有效。然而，由于与此类 3D 系统的 SFG 响应的理论计算相关的复杂性，SFG 特征的完整光谱解释一直很困难。本文描述了一种数值方法来预测 3D 系统中非中心对称纳米域的相对 SFG 强度，作为它们的大小和浓度以及它们的组装模式的函数，即倾斜、方位角和旋转角相对于实验室坐标。我们应用所开发的方法来预测与植物细胞壁结构相关的以各种顺序分布的结晶纤维素微纤维的 CH 和 OH 拉伸模式特征的变化。相同的算法也可以应用于散布在 3D 无定形基质中的任何 SFG 活性纳米域。我们应用所开发的方法来预测与植物细胞壁结构相关的以各种顺序分布的结晶纤维素微纤维的 CH 和 OH 拉伸模式特征的变化。相同的算法也可以应用于散布在 3D 无定形基质中的任何 SFG 活性纳米域。我们应用所开发的方法来预测与植物细胞壁结构相关的以各种顺序分布的结晶纤维素微纤维的 CH 和 OH 拉伸模式特征的变化。相同的算法也可以应用于散布在 3D 无定形基质中的任何 SFG 活性纳米域。

更新日期：2022-08-29

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