Identifying barriers to charge-carriers in the bulk and surface regions of Cu2ZnSnS4 nanocrystal films by x-ray absorption fine structures (XAFSs)

Turnbull, Matthew J.; Vaccarello, Daniel; Yiu, Yun Mui; Sham, Tsun-Kong; Ding, Zhifeng

doi:10.1063/1.4967863

Title: Identifying barriers to charge-carriers in the bulk and surface regions of Cu₂ZnSnS₄ nanocrystal films by x-ray absorption fine structures (XAFSs)

Journal Article · Tue Nov 22 00:00:00 EST 2016 · Journal of Chemical Physics

DOI:https://doi.org/10.1063/1.4967863· OSTI ID:1334802

Turnbull, Matthew J. ^[1]; Vaccarello, Daniel ^[1];

^[1]; Sham, Tsun-Kong ^[1]; Ding, Zhifeng ^[1]

Univ. of Western Ontario, London, ON (Canada). Dept. of Chemistry and Soochow Univ.-Western, Univ. Centre for Synchrotron Radiation Research

Solar cell performance is most affected by the quality of the light absorber layer. For thin-film devices, this becomes a two-fold problem of maintaining a low-cost design with well-ordered nanocrystal (NC) structure. The use of Cu₂ZnSnS₄ (CZTS) NCs as the light absorber films forms an ideal low-cost design, but the quaternary structure makes it difficult to maintain a well-ordered layer without the use of high-temperature treatments. There is little understanding of how CZTS NC structures affect the photoconversion efficiency, the charge-carriers, and therefore the performance of the device manufactured from it. To examine these relationships, the measured photoresponse from the photo-generation of charge-carrier electron-hole pairs was compared against the crystal structure, as short-range and long-range crystal orders for the films. The photoresponse simplifies the electronic properties into three basic steps that can be associated with changes in energy levels within the band structure. These changes result in the formation of barriers to charge-carrier flow. In this work, the extent of these barriers was determined using synchrotron-based X-ray absorbance fine structure to probe the individual metal centers in the film, and comparing these to molecular simulations of the ideal extended xray absorbance fine structure scattering. This allowed for the quantification of bond lengths, and thus an interpretation of the distortions in the crystal lattice. The various characteristics of the photoresponse were then correlated to the crystallographic order and used to gain physical insight into barriers to charge-carriers in the bulk and surface regions of CZTS films.

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Research Organization:: Argonne National Laboratory (ANL), Argonne, IL (United States). Advanced Photon Source (APS)

Sponsoring Organization:: USDOE Office of Science (SC), Basic Energy Sciences (BES). Scientific User Facilities Division; Natural Sciences and Engineering Research Council of Canada (NSERC)

Grant/Contract Number:: AC02-06CH11357

OSTI ID:: 1334802

Journal Information:: Journal of Chemical Physics, Vol. 145, Issue 20; ISSN 0021-9606

Publisher:: American Institute of Physics (AIP)Copyright Statement

Country of Publication:: United States

Language:: ENGLISH

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Title: Identifying barriers to charge-carriers in the bulk and surface regions of Cu₂ZnSnS₄ nanocrystal films by x-ray absorption fine structures (XAFSs)