Exploration on anion ordering, optical properties and electronic structure in K3WO3F3 elpasolite

• Published in: Journal of solid state chemistry 2012-03, Vol.187, p.159-164
• Main Authors: Atuchin, V.V., Isaenko, L.I., Kesler, V.G., Lin, Z.S., Molokeev, M.S., Yelisseyev, A.P., Zhurkov, S.A.
• Format: Article
• Language: English
• Subjects: Anions; Crystals; Electronic and optical properties; Electronic structure; Exploration; First-principles calculations; Forbidden bands; Mathematical analysis; Nonlinear optical crystals; Nonlinearity; Optical properties; Oxyfluorotungstate; Structure
• ISSN: 0022-4596; 1095-726X
• DOI: 10.1016/j.jssc.2011.12.037

Room-temperature modification of potassium oxyfluorotungstate, G2-K3WO3F3, has been prepared by low-temperature chemical route and single crystal growth. Wide optical transparency range of 0.3–9.4μm and forbidden band gap Eg=4.32eV have been obtained for G2-K3WO3F3 crystal. Meanwhile, its electronic structure has been calculated with the first-principles calculations. The good agreement between the theorectical and experimental results have been achieved. Furthermore, G2-K3WO3F3 is predicted to possess the relatively large nonlinear optical coefficients. Using the cm-size K3WO3F3 crystal (left upper), the transmission spectrum (right upper) and XPS valence electronic states (left lower) were measured, agreed with the ab initio results (right lower). [Display omitted] ► The cm-size G2-K3WO3F3 single crystals are obtained. ► Optical absorption edge and transmission range are defined for G2-K3WO3F3 crystal. ► Crystal structures of all known K3WO3F3 polymorph modifications are determined. ► Experimental electronic structure is consistent with the first-principles result. ► G2-K3WO3F3 is predicted as a crystal with large NLO coefficients.