Two-photon absorption and energy band structure of orthorhombic Hg2Cl2 crystals

Abstract

Dependence of two-photon absorption (TPA) rate on the state of polarization of a laser beam is investigated in the low-temperature orthorhombic modification of Hg2Cl2 crystals. Theoretical calculations of the dependence of TPA rate on the direction of polarization vector of the beam are performed for centrosymmetric pointsγ, Y, Z, T, R andS of the Brillouin zone. The domain structure of real crystals is taken into consideration and it is shown that periodicity of the polarization dependence may indicate whether TPA is due to transitions either atγ, Y, Z, T orR, S points. The polarization dependence of TPA cannot, however, distinguish between points inside these two groups. Comparison of theory with a low-temperature (T ∼ 8·5 K) experimental curve of polarization dependence is discussed. It is shown that the experiment can be explained in main features by a model of noninteracting oriented linear dipoles. Further, on the basis of TPA measurements, a simple energy band structure of Hg2Cl2 is proposed regarding Hg2Cl2 crystal as a linear chain of molecules.