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

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 points, 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 at, 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.The authors express thanks to Dr. . Barta for supplying the Hg₂Cl₂ crystals, Dr. Z. Bryknar for critical comments and Dr. B. Velický for stimulating discussion. We thank also Dr. V. Kohlová for assistance during measurement.