Synthesis, structure, linear and nonlinear optical properties of noncentrosymmetric quaternary diamond-like semiconductors, Cu2ZnGeSe4 (CZGSe) and the novel Cu4ZnGe2Se7

Sinagra, Charles W.; Saouma, Felix O.; Otieno, Calford O.; Lapidus, Saul H.; Zhang, Jian-Han; Craig, Andrew J.; Grima-Gallardo, Pedro; Brant, Jacilynn A.; Rosmus, Kimberly A.; Rosello, Kate E.; Jang, Joon I.; Aitken, Jennifer A.

doi:10.1016/j.jallcom.2021.161499

Title: Synthesis, structure, linear and nonlinear optical properties of noncentrosymmetric quaternary diamond-like semiconductors, Cu₂ZnGeSe₄ (CZGSe) and the novel Cu₄ZnGe₂Se₇

Journal Article · Thu Aug 19 00:00:00 EDT 2021 · Journal of Alloys and Compounds

DOI:https://doi.org/10.1016/j.jallcom.2021.161499· OSTI ID:1834616

Sinagra, Charles W. ^[1]; Saouma, Felix O. ^[2]; Otieno, Calford O. ^[3]; Lapidus, Saul H. ^[4]; Zhang, Jian-Han ^[5]; Craig, Andrew J. ^[1]; Grima-Gallardo, Pedro ^[6]; Brant, Jacilynn A. ^[1]; Rosmus, Kimberly A. ^[1]; Rosello, Kate E. ^[1]; Jang, Joon I. ^[7]; Aitken, Jennifer A. ^[1]

Duquesne Univ., Pittsburgh, PA (United States)
Kaimosi Friends University College (Kenya)
Kissi Universtiy (Kenya)
Argonne National Lab. (ANL), Argonne, IL (United States)
Sanming University (China)
Universidad de Los Andes (ULA), Merida (Venezuela); Centro Nacional de Tecnologia Optica (CNTO), Merida (Venezuela)
Sogang University, Seoul (Korea, Republic of)

In this work, two quaternary diamond-like semiconductors (DLSs) in the Cu-Zn-Ge-Se system, the known Cu₂ZnGeSe₄ (also referred to as CZGSe) and the new Cu₄ZnGe₂Se₇, are compared in terms of their crystal structures, electronic structures and physicochemical properties. Both compounds were prepared by high-temperature, solid-state synthesis at 800 degrees C. Single crystal X-ray diffraction was used to determine the structure of Cu₄ZnGe₂Se₇. The structures of both Cu₂ZnGeSe₄ and Cu₄ZnGe₂Se₇ can be considered as derivatives of cubic diamond. Cu₄ZnGe₂Se₇, with a reduced symmetry due to the cation ordering pattern, adopts the Cu₄NiSi₂S₇ structure type, with space group C2. The corner-sharing tetrahedra in Cu₄ZnGe₂Se₇ are slightly distorted because the charge for some of the S²- anions is not compensated by the first-nearest-neighbor cations. Rietveld refinements using synchrotron X-ray powder diffraction data were used to assess the phase purity of the samples and confirm the bulk structural behavior. Diffuse reflectance UV/Vis/NIR spectroscopy shows that Cu₂ZnGeSe₄ and Cu₄ZnGe₂Se₇ have direct optical bandgaps of 1.38 and 0.91 eV, respectively. Electronic structure calculations implementing density functional theory confirm the direct bandgap for Cu₄ZnGe₂Se₇, with a calculated value of 0.62 eV. Both compounds are air stable, thermally stable up to relatively high temperatures, undergo phase transitions and have wide windows of optical clarity. The Kurtz-Perry powder technique was used to determine the second harmonic generation (SHG) responses using a commercial AgGaSe₂ standard. While Cu₄ZnGe₂Se₇ displays a weak SHG response, Cu₂ZnGeSe₄ exhibits a response that is greater than several benchmark materials, with a large SHG coefficient, χ⁽²⁾, of 43 ± 6 pm/V at λ = 2900 nm.

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Research Organization:: Argonne National Lab. (ANL), Argonne, IL (United States)

Sponsoring Organization:: USDOE Office of Science (SC), Basic Energy Sciences (BES); National Science Foundation (NSF); National Research Foundation of Korea (NRF)

Grant/Contract Number:: AC02-06CH11357; DMR-1201729; DMR-1611198; CHE-0234872; DUE-0511444; 2017R1D1A1B03035539; 2020R1F1A1069646

OSTI ID:: 1834616

Journal Information:: Journal of Alloys and Compounds, Vol. 888; ISSN 0925-8388

Publisher:: ElsevierCopyright Statement

Country of Publication:: United States

Language:: English

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Title: Synthesis, structure, linear and nonlinear optical properties of noncentrosymmetric quaternary diamond-like semiconductors, Cu₂ZnGeSe₄ (CZGSe) and the novel Cu₄ZnGe₂Se₇