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首页> 外文期刊>The journal of physical chemistry, A. Molecules, spectroscopy, kinetics, environment, & general theory >Quantitative orientation analysis by sum frequency generation in the presence of near-resonant background signal: Acetonitrile on rutile TiO _2 (110)
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Quantitative orientation analysis by sum frequency generation in the presence of near-resonant background signal: Acetonitrile on rutile TiO _2 (110)

机译：在近共振背景信号：金红石TiO _2（110）上存在乙腈时，通过和频产生的定量取向分析

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摘要

Sum frequency generation (SFG) spectroscopic techniques are used to investigate the molecular orientation of adsorbed acetonitrile on rutile TiO_2 (110) at the solid-vapor interface. Generally, most molecular orientation analyses using SFG have been performed on dielectric substrates, to avoid the spectral interference between resonant and the near-resonant background signal. Although rutile crystal can be treated as a dielectric substrate, its electronic state contributes to the intensity and interferes with the resonant signal when the SFG frequency is close to its band gap energy. In addition, the rutile crystal is a uniaxial birefringent material, and the (110) surface is anisotropic, which further complicates the spectral analysis. In this study, various SFG measurement techniques were applied, and quantitative analytical methods were established to interpret the surface orientation of an adsorbed molecule. SFG vibrational spectra of acetonitrile on rutile TiO _2 (110) surface have been measured using distinct polarization combinations, polarization mapping, and null angle method. By varying the polarization combinations of SFG, the magnitude and shape of the spectra undergo substantial change, which originate from the interference between the near-resonant signal from the rutile substrate and the resonance signal from the acetonitrile. Theory, simulation, and analytical methods for obtaining quantitative orientation information of a molecule on an anisotropic semiconductor substrate in the presence of a near-resonant signal are presented.
机译：总和频率产生（SFG）光谱技术用于研究固-金红石界面上金红石TiO_2（110）上吸附的乙腈的分子取向。通常，大多数使用SFG的分子取向分析都是在介电基片上进行的，以避免共振和近共振背景信号之间发生光谱干扰。尽管可以将金红石晶体用作介电基片，但当SFG频率接近其带隙能量时，其电子态有助于强度并干扰谐振信号。此外，金红石晶体是单轴双折射材料，并且（110）表面是各向异性的，这进一步使光谱分析复杂化。在这项研究中，应用了各种SFG测量技术，并建立了定量分析方法来解释吸附分子的表面取向。使用不同的极化组合，极化映射和零角法测量了金红石TiO _2（110）表面上乙腈的SFG振动光谱。通过改变SFG的偏振组合，光谱的大小和形状会发生实质性变化，这是由于来自金红石基质的近共振信号与来自乙腈的共振信号之间的干扰引起的。提出了在近共振信号存在下获得各向异性半导体衬底上分子定量取向信息的理论，模拟和分析方法。

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