Exploration of Electrostatic Field Force in Surface-Enhanced Raman Scattering: An Experimental Investigation Aided by Density Functional Calculations

拉曼散射 化学 密度泛函理论 化学物理 胶体金 分子 纳米颗粒 化学吸附 拉曼光谱 分析物 胶体 纳米技术 计算化学 吸附 材料科学 物理化学 有机化学 光学 物理
作者
Sougata Sarkar,Surojit Pande,Subhra Jana,Arun K. Sinha,Mukul Pradhan,Mrinmoyee Basu,Joydeep Chowdhury,Tarasankar Pal
出处
期刊:Journal of Physical Chemistry C [American Chemical Society]
卷期号:112 (46): 17862-17876 被引量:32
标识
DOI:10.1021/jp804028w
摘要

Surface chemical properties of metal nanoparticles must be tunable to create chemical specificity and are a key prerequisite for successful sensing and imaging platforms. To relate surface enhanced Raman scattering (SERS) to electrostatic field force, a simple colloidal chemistry approach has been deliberately exploited for syntheses of gold nanoparticles with negative and positive surface charges to study their interactions with charged analytes. We took up the challenge with sulfur-containing analytes because "Au−S" interaction is well-known. Thiocyanate ion, −SCN−, a well-known SERS analyte, has been proved to be chemically ligated/anchored on positively charged gold nanoparticles surface owing to favorable electrostatic attraction. The Au−S vibrational band at ∼240 cm−1 and blue-shifting of the −C≡N stretching frequency by ∼46 cm−1 in conjunction with its intensity enhancement by an order of ∼103 in the SERS spectrum clearly illustrate a chemisorption phenomenon. In contrast, physisorption of the −SCN− ion becomes evident on negatively charged colloid. Again, methylene blue has been shown to remain engrossed on the negatively charged gold surfaces. However, the electrostatic field force could not be accounted for from fluorescence quenching while methylaminopyrene was introduced because of the distance-dependence effect. The feasibility of such coordinative/chemical attachment also has been examined theoretically by density functional theory (DFT). Moreover, employment of this DFT calculation has been performed on five different metal−molecule interaction models to fruitfully interpret the experimental SERS findings and also the orientation of the SERS analyte. The observed Raman signals have been assigned from the potential energy distributions in terms of internal coordinates of adsorbate from the output of DFT calculations. The results thus provide a benchmark illustration of the value of DFT for aiding interpretation of adsorbate vibrational spectra attainable by using SERS.
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