Na{sub 2}Ge{sub 2}Se{sub 5}: A highly nonlinear optical material
- Department of Chemistry, Northwestern University, Evanston, IL 60208 (United States)
- Department of Physics and Astronomy, Northwestern University, Evanston, IL 60208 (United States)
We report an integrated experimental and theoretical study of the two-dimensional polar selenogermanate compound Na{sub 2}Ge{sub 2}Se{sub 5}, which exhibits strong nonlinear optical (NLO) second harmonic generation response in the visible and infrared region. The compound is type-I phase-matchable with a large SHG coefficient {chi}{sup (2)} Almost-Equal-To 290 pm V{sup -1}, which is the second highest among the phase-matchable NLO materials. It also performs as an NLO frequency mixer to produce radiation via difference frequency generation. The compound is optically transparent from the visible (0.521 {mu}m) to the far IR (18.2 {mu}m) and melts congruently. Ab initio density functional theory band structure calculations show that the unusually large second-order optical nonlinearity is attributed to the two-dimensional character of the crystal structure. Raman, IR and optical absorption spectroscopy, differential thermal analysis, NLO properties of derivatives of Na{sub 2}Ge{sub 2}Se{sub 4.55}Te{sub 0.45} and Na{sub 2}Ge{sub 1.64}Sn{sub 0.36}Se{sub 5} and thermal expansion behavior studies are also reported. - Graphical Abstract: Na{sub 2}Ge{sub 2}Se{sub 5} is a new second-order nonlinear optical material for IR applications. It is type-I phase-matchable with a large SHG coefficient {chi}{sup (2)} Almost-Equal-To 290 pm V{sup -1}, which is the second largest among the phase-matchable NLO materials. Highlights: Black-Right-Pointing-Pointer Na{sub 2}Ge{sub 2}Se{sub 5} is a new second-order nonlinear optical material for IR applications. Black-Right-Pointing-Pointer It is type-I phase-matchable. Black-Right-Pointing-Pointer Its SHG coefficient {chi}{sup (2)} Almost-Equal-To 290 pm V{sup -1} is the second largest among the phase-matchable NLO materials. Black-Right-Pointing-Pointer Its DFG performance allows the development of a multiple IR frequency source with tunability. Black-Right-Pointing-Pointer Ab initio density functional theory band structure calculations show that the unusually large second-order optical nonlinearity is attributed to the 2-D character of the crystal structure.
- OSTI ID:
- 22149900
- Journal Information:
- Journal of Solid State Chemistry, Vol. 195; Other Information: Copyright (c) 2012 Elsevier Science B.V., Amsterdam, The Netherlands, All rights reserved.; Country of input: International Atomic Energy Agency (IAEA); ISSN 0022-4596
- Country of Publication:
- United States
- Language:
- English
Similar Records
New nonlinear optical potassium iodate K[IO{sub 3}] and borates K{sub 3}[B{sub 6}O{sub 10}]Br, KTa[B{sub 4}O{sub 6}(OH){sub 4}](OH){sub 2}{center_dot}1.33H{sub 2}O-Synthesis, structures and relation to the properties
Structure and optical properties of a noncentrosymmetric borate RbSr{sub 4}(BO{sub 3}){sub 3}