title: Identifying barriers to charge-carriers in the bulk and surface regions of Cu2ZnSnS4nanocrystal films by x-ray absorption fine structures (XAFSs).
abstract: 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. 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 x-ray 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.
authors.affiliation: Department of Chemistry and Soochow University-Western, University Centre for Synchrotron Radiation Research, The University of Western Ontario, 1151 Richmond Street, London, Ontario N6A 5B7, Canada.
authors.forename: Matthew J
authors.initials: MJ
authors.lastname: Turnbull
authors.affiliation: Department of Chemistry and Soochow University-Western, University Centre for Synchrotron Radiation Research, The University of Western Ontario, 1151 Richmond Street, London, Ontario N6A 5B7, Canada.
authors.forename: Daniel
authors.initials: D
authors.lastname: Vaccarello
authors.affiliation: Department of Chemistry and Soochow University-Western, University Centre for Synchrotron Radiation Research, The University of Western Ontario, 1151 Richmond Street, London, Ontario N6A 5B7, Canada.
authors.forename: Yun Mui
authors.initials: YM
authors.lastname: Yiu
authors.affiliation: Department of Chemistry and Soochow University-Western, University Centre for Synchrotron Radiation Research, The University of Western Ontario, 1151 Richmond Street, London, Ontario N6A 5B7, Canada.
authors.forename: Tsun-Kong
authors.initials: TK
authors.lastname: Sham
authors.affiliation: Department of Chemistry and Soochow University-Western, University Centre for Synchrotron Radiation Research, The University of Western Ontario, 1151 Richmond Street, London, Ontario N6A 5B7, Canada.
authors.forename: Zhifeng
authors.initials: Z
authors.lastname: Ding