Klanjšek-Gunde Marta, Ivanovski Vladimir, Orel Boris
Acta Chim Slov. 2011 Sep;58(3):528-41.
Reflectance spectra may show very different and interesting shapes. The most interesting may be connected to Evans holes. Model calculations to reproduce this effect were done applying model dielectric function functions. When a weak oscillator appears within the frequency region of a strong one (i.e. between its TO and LO frequencies), its LO-mode frequency shifts towards higher wavenumbers. As a consequence, the oscillator strength of the corresponding weak mode becomes negative which produces a dip (Evans hole) in the reflectance spectrum. This model was successfully applied to analyze polarized reflectance spectra of potassium hydrogen succinate monocrystal in the ac crystal plane. The crystal symmetry was described by phenomenological model and by full symmetry consideration. The phenomenological approach applies the four-parametric model for dielectric function which allows good evaluation of asymmetric reflectance bands. A cosine dependence of oscillator strength on polarization angle was obtained for some bands, most likely due to small deviation of the crystal symmetry from orthorhombic. This is why the phenomenological approach provides good parameters for almost all phonon modes. The full symmetry consideration applies real description of dielectric tensor in the ac plane and the three-parameter model for dielectric function. This model could give very accurate directions of transition dipole moments, but cannot fit asymmetric bands well to measured reflectance. Both approaches describe all basic spectral features, the wide reflectance of asOH and the two Evans holes appearing on its shoulder.
反射光谱可能呈现出非常不同且有趣的形状。最有趣的可能与埃文斯空穴有关。为了重现这种效应,我们应用模型介电函数进行了模型计算。当一个弱振子出现在一个强振子的频率区域内(即在其横向光学(TO)频率和纵向光学(LO)频率之间)时,其LO模式频率会向更高波数移动。结果,相应弱模式的振子强度变为负值,这在反射光谱中产生一个凹陷(埃文斯空穴)。该模型已成功应用于分析琥珀酸氢钾单晶在交流晶体平面中的偏振反射光谱。晶体对称性通过唯象模型和完全对称性考虑来描述。唯象方法应用四参数介电函数模型,该模型能够很好地评估不对称反射带。对于某些谱带,得到了振子强度与偏振角的余弦依赖关系,这很可能是由于晶体对称性与正交晶系存在小偏差。这就是为什么唯象方法能为几乎所有声子模式提供良好参数的原因。完全对称性考虑应用了交流平面中介电张量的真实描述以及介电函数的三参数模型。该模型能够给出非常准确的跃迁偶极矩方向,但不能很好地将不对称谱带拟合到测量的反射率上。两种方法都描述了所有基本光谱特征,即asOH的宽反射以及出现在其肩部的两个埃文斯空穴。