理论研究Ag/MPH/TiO2体系的SERS光谱化学增强机理

doi:10.3866/PKU.WHXB20110602

Abstract

Abstract:

A chemically enhanced mechanism of surface-enhanced Raman scattering (SERS) spectroscopy was investigated using density functional theory (DFT). We studied the Raman spectra of the Ag₁₃/MPH and Ag₁₃/MPH/TiO₂ systems under 514.5 nm excitation. We found that the intensities of the non-totally symmetric vibration modes were selectively enhanced after TiO₂ was introduced into the Ag₁₃/MPH system. By analyzing the ground state and excited states of the charge transfer (CT) complex we found that the system gave a photoinduced CT state from Ag to the MPH-TiO₂ complex when the excitation wavelength exceeded the optical absorption threshold (635 nm) of the MPH-TiO₂ complex. The selective enhancement of the b₂ modes in the SERS spectra probably originates from the Herzberg-Teller mechanism through the coupling of the corresponding modes with the CT transition. Our theoretical results support the experimental results and also define the adsorption threshold of the CT complex clearly while providing an intelligible physical explanation for the laser wavelength-dependent SERS phenomenon.

Key words: Surface-enhanced Raman scattering, Density functional theory, Charge transfer complex, Chemically enhanced mechanism

SUN Lei, BAI Fu-Quan, ZHANG Hong-Xing. Theoretical Investigation of Chemically Enhanced Mechanism of SERS Spectroscopy for Ag/MPH/TiO₂ System[J]. Acta Phys. -Chim. Sin. 2011, 27(06), 1335-1340. doi: 10.3866/PKU.WHXB20110602

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Theoretical Investigation of Chemically Enhanced Mechanism of SERS Spectroscopy for Ag/MPH/TiO₂ System

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Theoretical Investigation of Chemically Enhanced Mechanism of SERS Spectroscopy for Ag/MPH/TiO₂ System