Understanding of nonlinear optical properties of CS _2 from a microscopic viewpoint

摘要

This study is to improve understanding of nonlinear optics through investigating the microstructures of carbon disulfide (CS _2) liquid, an important nonlinear optical material. First principles methods are employed in this work to investigate the structure, vibrational spectra, and the 2nd hyperpolarizabilites of CS _2 clusters up to tetramers. Three types of molecular arrangements of clusters with different sizes are identified. The cluster conformations are prone to inter-converting under external disturbance due to the weak interactions among molecules. The correlation between the nonlinear optical properties and the conformation of CS _2 clusters are studied in detail in this work.