论文标题
计算拉曼信号超出diatomic分子晶体的扰动理论
Calculating the Raman Signal Beyond Perturbation Theory for a Diatomic Molecular Crystal
论文作者
论文摘要
我们在一系列模型均值势范围内计算了双原子分子的本征状状态,并评估其相关拉曼光谱与场强的演变。我们证明,硅藻分子的拉曼光谱外观发生了巨大变化,而周围电位的对称性没有任何相关的变化。从经典的意义上讲,量子本征的限制案例对应于自由旋转和定向分子的库。但是,也有许多混合模式既不是rotons也不是图书馆。拉曼光谱的后果是一系列并发症 - 非谐波电位将拉曼活跃模式分开,并打破了禁止模式的选择规则。各种状态的质量依赖性不同 - 转子,振荡器和重新定向的$ 1/m $,$ 1/\ sqrt {m} $和较弱的质量依赖性。这可能使人们可以通过同位素光谱识别该模式的特征。然而,混合模式和具有不同特征的两个不同特征状态之间的过渡使它变得复杂。我们得出的结论是,分子系统的拉曼频谱的显着变化不足以证明相变,因为这种变化在增加场强度时也可以在固定的对称潜力中发生。
We calculate the eigenstates of a diatomic molecule in a range of model mean-field potentials, and evaluate the evolution of their associated Raman spectra with field strength. We demonstrate that dramatic changes in the appearance of the Raman spectrum for a diatomic molecule occur without any associated change in the symmetry of the surrounding potential. The limiting cases of the quantum eigenstates correspond, in the classical sense, to free rotation, and libration of well-oriented molecules. However, there are also many mixed modes which are neither rotons nor librons. The consequence for Raman spectroscopy is a series of complications - the non-harmonic potential splits the Raman active modes, and breaks the selection rules on forbidden modes. The mass-dependence of the various states is different - rotors, oscillators and reorientations have $1/m$, $1/\sqrt{m}$ and weaker mass dependence respectively. This may allow one to identify the character of the mode with isotope spectroscopy. However it is complicated by mixed modes and transitions between two different eigenstates with different character. We conclude that significant changes in the Raman spectrum of molecular systems are insufficient to demonstrate a phase transition since such changes can also occur in a fixed symmetry potential upon increasing field strength.