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) = 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.
- OSTI ID:
- 22420553
- Journal Information:
- Materials Research Bulletin, Vol. 57; Other Information: Copyright (c) 2014 Elsevier Science B.V., Amsterdam, The Netherlands, All rights reserved.; Country of input: International Atomic Energy Agency (IAEA); ISSN 0025-5408
- Country of Publication:
- United States
- Language:
- English
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Related Subjects
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