Simulating Ensemble-Averaged Surface-Enhanced Raman Scattering
Simulating Ensemble-Averaged Surface-Enhanced Raman Scattering
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DOI：
10.1021/acs.jpcc.6b02159
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发表时间：
2016-09-22
影响因子：
3.7
通讯作者：
Jensen, Lasse
中科院分区：
文献类型：
--
作者：
Chulhai, Dhabih V.;Chen, Xing;Jensen, Lasse
模拟表面增强拉曼散射（Sers）的能力是阐明等离子体金属纳米颗粒附近分子化学性质的重要工具。然而，典型的方法不包括感兴趣的分子的动力学，并且通常限于单个或几个分子。在这项工作中，我们结合联合收割机分子动力学模拟与dressed张量形式主义，模拟Sers光谱的银纳米粒子涂有一个完整的单层吡啶分子。该方法允许：我们模拟更现实的大规模系统的整体平均Sers光谱，同时考虑到热点中分子的组织。通过这些模拟，我们发现，优先，结合的位置和方向的分子，选择电动力学方法，并列入场梯度效应的影响增强分布和光谱特征。我们还表明，通过其Sers光谱可以有效地跟踪纳米颗粒交界处附近的吡啶分子的平移和旋转运动。
The ability to simulate surface-enhanced Raman scattering (SERS) is a vital tool in elucidating the chemistry of molecules near the vicinity of plasmonic metal nanoparticles. However, typical methods do not include the dynamics of the molecule(s) of interest and are often limited to a single or few molecules. In this work, we combine molecular dynamics simulations with the dressed-tensor formalism to simulate the SERS spectra-of Ag nanoparticles coated with a full monolayer of pyridine molecules. This method allows: us to simulate the ensemble-averaged SERS spectra of more realistic large scale systems, while accounting for the organization of molecules in the hotspots. Through these simulations, we find that the preferential, binding location and orientation of the molecules,: the choice of electrodynamics Method, and the inclusion of field gradient effects influence both the enhancement distribution and the spectral signatures. We also show that both the translational and rotational motions of a pyridine molecule near a nanoparticle junction may be effectively tracked through its SERS spectrum.