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Title: Na{sub 2}Ge{sub 2}Se{sub 5}: A highly nonlinear optical material

Abstract

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{submore » 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.« less

Authors:
 [1]; ; ;  [2];  [1]
  1. Department of Chemistry, Northwestern University, Evanston, IL 60208 (United States)
  2. Department of Physics and Astronomy, Northwestern University, Evanston, IL 60208 (United States)
Publication Date:
OSTI Identifier:
22149900
Resource Type:
Journal Article
Journal Name:
Journal of Solid State Chemistry
Additional Journal Information:
Journal Volume: 195; Other Information: Copyright (c) 2012 Elsevier Science B.V., Amsterdam, The Netherlands, All rights reserved.; Country of input: International Atomic Energy Agency (IAEA); Journal ID: ISSN 0022-4596
Country of Publication:
United States
Language:
English
Subject:
36 MATERIALS SCIENCE; ABSORPTION SPECTROSCOPY; CHALCOGENIDES; CRYSTAL STRUCTURE; DENSITY FUNCTIONAL METHOD; DIFFERENTIAL THERMAL ANALYSIS; HARMONIC GENERATION; NONLINEAR OPTICS; NONLINEAR PROBLEMS; SEMICONDUCTOR MATERIALS; TWO-DIMENSIONAL CALCULATIONS

Citation Formats

Chung, In, Song, Jung-Hwan, Jang, Joon I., Freeman, Arthur J., and Kanatzidis, Mercouri G., E-mail: m-kanatzidis@northwestern.edu. Na{sub 2}Ge{sub 2}Se{sub 5}: A highly nonlinear optical material. United States: N. p., 2012. Web. doi:10.1016/J.JSSC.2012.05.038.
Chung, In, Song, Jung-Hwan, Jang, Joon I., Freeman, Arthur J., & Kanatzidis, Mercouri G., E-mail: m-kanatzidis@northwestern.edu. Na{sub 2}Ge{sub 2}Se{sub 5}: A highly nonlinear optical material. United States. doi:10.1016/J.JSSC.2012.05.038.
Chung, In, Song, Jung-Hwan, Jang, Joon I., Freeman, Arthur J., and Kanatzidis, Mercouri G., E-mail: m-kanatzidis@northwestern.edu. Thu . "Na{sub 2}Ge{sub 2}Se{sub 5}: A highly nonlinear optical material". United States. doi:10.1016/J.JSSC.2012.05.038.
@article{osti_22149900,
title = {Na{sub 2}Ge{sub 2}Se{sub 5}: A highly nonlinear optical material},
author = {Chung, In and Song, Jung-Hwan and Jang, Joon I. and Freeman, Arthur J. and Kanatzidis, Mercouri G., E-mail: m-kanatzidis@northwestern.edu},
abstractNote = {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.},
doi = {10.1016/J.JSSC.2012.05.038},
journal = {Journal of Solid State Chemistry},
issn = {0022-4596},
number = ,
volume = 195,
place = {United States},
year = {2012},
month = {11}
}