journal article·2019-10-22Open access

Tuning Electrical, Optical, and Thermal Properties through Cation Disorder in Cu2ZnSnS4

Kevin Ye, Sin Cheng Siah, Peter T. Erslev, Austin Akey, Charles Settens, Md Shafkat Bin Hoque, Jeffrey Braun, Patrick Hopkins, Glenn Teeter, Tonio Buonassisi, R. Jaramillo

Chemistry of Materials· Volume 31· Issue 20

Abstract

Chemical disorder in semiconductors is important to characterize reliably because it affects materials performance, for instance by introducing potential fluctuations and recombination sites. It also represents a means to control material properties, to far exceed the limits of equilibrium thermodynamics. We present a study of highly disordered Cu–Zn–Sn–S (d-CZTS) films along the Cu2SnS3–Cu2ZnSnS4–ZnS binary line, deposited by physical vapor deposition. Deposition at low temperature kinetically stabilizes compositions that are well outside of the narrow, equilibrium solid solution of kesterite (Cu2ZnSnS4). Here we study d-CZTS and its thermal treatment using complementary characterization techniques: X-ray absorption spectroscopy (XAS), X-ray diffraction (XRD), and transmission electron microscopy (TEM). We find that cations in d-CZTS are highly disordered while the sulfur anions remain in a well-defined, cubic close-packed lattice. On the atomic scale, composition fluctuations are accommodated preferentially by stacking faults. Kinetically-stabilized cation disorder can produce nonequilibrium semiconductor alloys with a wide range of band gap, electronic conductivity, and thermal conductivity. d-CZTS therefore represents a processing route to optimizing materials for optoelectronic device elements such as light absorbers, window layers, and thermal barriers.
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Research context

OpenAlex topics: Chalcogenide Semiconductor Thin Films · Quantum Dots Synthesis And Properties · Copper-based nanomaterials and applications

SciVX discovery tags are terminology-based. OpenAlex topics are source-provided classifications.

Affiliations

Department of Materials Science and Engineering, Massachusetts Institute of Technology, 77 Massachusetts Avenue, Cambridge, Massachusetts 02139, United States

Department of Mechanical Engineering, Massachusetts Institute of Technology, 77 Massachusetts Avenue, Cambridge, Massachusetts 02139, United States

National Center for Photovoltaics, National Renewable Energy Laboratory, 15013 Denver West Parkway, Golden, Colorado 80401, United States

Center for Nanoscale Systems, Harvard University, Cambridge, Massachusetts 02138, United States

Materials Research Laboratory, Massachusetts Institute of Technology, 77 Massachusetts Avenue, Cambridge, Massachusetts 02139, United States

Department of Mechanical and Aerospace Engineering, University of Virginia, Charlottesville, Virginia 22904, United States

Department of Materials Science and Engineering, University of Virginia, Charlottesville, Virginia 22904, United States

Department of Physics, University of Virginia, Charlottesville, Virginia 22904, United States

Funding

Army Research Office · Office of Energy Efficiency and Renewable Energy · National Renewable Energy Laboratory

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