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Title: Growth and characterization of kesterite Cu{sub 2}ZnSn(S{sub x}Se{sub 1−x}){sub 4} crystals for photovoltaic applications

Highlights: • Cu{sub 2}ZnSn(S{sub x}Se{sub 1−x}){sub 4} crystals were grown using vertical gradient freeze technique. • Grown CZTSSe crystals exhibited highly crystalline tetragonal kesterite structure. • Grown ingot showed a homogeneous, stoichiometric composition along the growth axis. • Cu-rich particulates were observed along the polycrystalline grain boundaries. • Large volume of high quality CZTSSe can be grown using this novel VGF method. - Abstract: Cu{sub 2}ZnSn(S{sub x}Se{sub 1−x}){sub 4} (CZTSSe) bulk crystals have been grown for the first time, in multi-gram quantities, using a novel vertical gradient freeze (VGF) technique. Large grain polycrystalline CZTSSe ingot with grain sizes ∼0.2–0.5 mm was grown in a vacuum sealed quartz ampoule. Structural, compositional, and electronic properties of the ingot were characterized by X-ray diffraction (XRD), X-ray photoelectron spectroscopy (XPS), energy dispersive X-ray spectroscopy (EDS), and van der Pauw measurements. XRD analysis showed highly crystalline tetragonal structure corresponding to kesterite CZTSSe with lattice constants of a = 5.563 Å, and c = 11.09 Å (c/2a = 0.997) and Raman spectra confirmed the formation of single phase CZTSSe. High-resolution XPS spectra confirmed the formation of metal-sulfoselenides. The ingot along the growth axis showed a homogeneous near stoichiometric elemental distribution corresponding to Cu/(Zn + Sn) =more » 0.94 and Zn/Sn = 0.98. EDS mapping on the ingot's outer surface revealed formation of islanded Cu-rich droplets at the grain boundaries. Grown crystals exhibited p-type conductivity with a measured bulk resistivity of ∼51 Ω cm.« less
Authors:
;
Publication Date:
OSTI Identifier:
22420553
Resource Type:
Journal Article
Resource Relation:
Journal Name: Materials Research Bulletin; Journal Volume: 57; Other Information: Copyright (c) 2014 Elsevier Science B.V., Amsterdam, The Netherlands, All rights reserved.; Country of input: International Atomic Energy Agency (IAEA)
Country of Publication:
United States
Language:
English
Subject:
36 MATERIALS SCIENCE; CONCENTRATION RATIO; COPPER COMPOUNDS; CRYSTAL GROWTH; GRAIN BOUNDARIES; GRAIN SIZE; LATTICE PARAMETERS; PARTICULATES; PHOTOVOLTAIC EFFECT; POLYCRYSTALS; QUARTZ; RAMAN SPECTRA; SEMICONDUCTOR MATERIALS; STOICHIOMETRY; SURFACES; TIN SELENIDES; X-RAY DIFFRACTION; X-RAY PHOTOELECTRON SPECTROSCOPY; X-RAY SPECTROSCOPY; ZINC SULFIDES