Resonance Raman and polarized Raman scattering of single‐crystal hematite

拉曼散射 拉曼光谱 X射线拉曼散射 化学 共振(粒子物理) 散射 声子 赤铁矿 激发 相干反斯托克斯拉曼光谱 偶极子 极化(电化学) 分子物理学 原子物理学 凝聚态物理 光学 物理 矿物学 有机化学 量子力学 物理化学
作者
Craig P. Marshall,William J.B. Dufresne
出处
期刊:Journal of Raman Spectroscopy [Wiley]
卷期号:53 (5): 947-955 被引量:10
标识
DOI:10.1002/jrs.6309
摘要

Abstract Researchers have demonstrated that the Raman spectra collected on hematite nanoparticles undergo an intensity enhancement, due to a dependence on excitation energy. Especially, the bands at approximately 660 and approximately 1320 cm −1 , which are assigned as the 1LO and 2LO modes, respectively, experience the strongest intensity enhancement, which has been attributed to resonance Raman scattering when excited with excitation energy at or close to the band gap. However, the resonance Raman scattering mechanism is not clear and further has not been experimentally determined. To this end, we have undertaken measurements to examine the excitation energy dependence and polarized Raman scattering on a pure single‐crystal of hematite to gain a better understanding of the resonance enhancement mechanism for the 1LO and 2LO modes. Resonance enhancement mechanisms giving rise to LO phonons in semiconductors can be attributed to either the deformation potential (DP) or Fröhlich interactions (F) scattering, or a combination of the two. The DP and F contributions that give rise to LO phonon scattering in semiconductors are distinguishable due to their contrasting selection rules. Here, employing these selection rules, we conducted the following polarization Raman scattering measurements: , , , , , , and on single‐crystal hematite to distinguish between DP (dipole‐allowed) and F (dipole‐forbidden) scattering. Our polarization experiments strongly suggest that the Fröhlich LO phonon interaction dominates the Raman scattering over the weaker DP contribution. Furthermore, polarization experiments collected using the following geometries and demonstrate that the interference between dipole‐allowed and dipole‐forbidden Raman scattering is constructive for LO phonons. Therefore, we attribute the mechanism of resonance Raman scattering of the 1LO and 2LO modes in the Raman spectrum of hematite due to contributions from F and DP processes.
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