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Title: The role of interparticle heterogeneities in the selenization pathway of Cu-Zn-Sn-S nanoparticle thin films: A real-time study

Real-time energy dispersive x-ray diffraction (EDXRD) analysis has been utilized to observe the selenization of Cu-Zn-Sn-S nanoparticle films coated from three nanoparticle populations: Cu- and Sn-rich particles roughly 5 nm in size, Zn-rich nanoparticles ranging from 10 to 20 nm in diameter, and a mixture of both types of nanoparticles (roughly 1:1 by mass), which corresponds to a synthesis recipe yielding CZTSSe solar cells with reported total-area efficiencies as high as 7.9%. The EDXRD studies presented herein show that the formation of copper selenide intermediates during the selenization of mixed-particle films can be primarily attributed to the small, Cu- and Sn-rich particles. Moreover, the formation of these copper selenide phases represents the first stage of the CZTSSe grain growth mechanism. The large, Zn-rich particles subsequently contribute their composition to form micrometer-sized CZTSSe grains. In conclusion, these findings enable further development of a previously proposed selenization pathway to account for the roles of interparticle heterogeneities, which in turn provides a valuable guide for future optimization of processes to synthesize high quality CZTSSe absorber layers.
Authors:
 [1] ;  [2] ;  [1] ;  [1] ;  [2] ;  [2] ;  [2] ;  [2] ;  [1] ;  [3] ;  [4] ;  [2] ;  [1]
  1. Purdue Univ., West Lafayette, IN (United States)
  2. Helmholtz-Zentrum Berlin fur Materialien und Energie, Berlin (Germany)
  3. Helmholtz-Zentrum Berlin (HZB), (Germany). German Research Centre for Materials and Energy
  4. Brookhaven National Lab. (BNL), Upton, NY (United States)
Publication Date:
Report Number(s):
BNL-108311-2015-JA
Journal ID: ISSN 2050-7526; KC0403020
Grant/Contract Number:
SC00112704
Type:
Accepted Manuscript
Journal Name:
Journal of Materials Chemistry. C
Additional Journal Information:
Journal Volume: 3; Journal Issue: 27; Journal ID: ISSN 2050-7526
Publisher:
Royal Society of Chemistry
Research Org:
Brookhaven National Laboratory (BNL), Upton, NY (United States)
Sponsoring Org:
USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22)
Country of Publication:
United States
Language:
English
Subject:
36 MATERIALS SCIENCE; Center for Functional Nanomaterials
OSTI Identifier:
1214519

Carter, Nathaniel J., Mainz, Roland, Walker, Bryce C., Hages, Charles J., Just, Justus, Klaus, Manuela, Schmidt, Sebastian S., Weber, Alfons, Yang, Wei -Chang D., Zander, Ole, Stach, Eric A., Unold, Thomas, and Agrawal, Rakesh. The role of interparticle heterogeneities in the selenization pathway of Cu-Zn-Sn-S nanoparticle thin films: A real-time study. United States: N. p., Web. doi:10.1039/C5TC01139F.
Carter, Nathaniel J., Mainz, Roland, Walker, Bryce C., Hages, Charles J., Just, Justus, Klaus, Manuela, Schmidt, Sebastian S., Weber, Alfons, Yang, Wei -Chang D., Zander, Ole, Stach, Eric A., Unold, Thomas, & Agrawal, Rakesh. The role of interparticle heterogeneities in the selenization pathway of Cu-Zn-Sn-S nanoparticle thin films: A real-time study. United States. doi:10.1039/C5TC01139F.
Carter, Nathaniel J., Mainz, Roland, Walker, Bryce C., Hages, Charles J., Just, Justus, Klaus, Manuela, Schmidt, Sebastian S., Weber, Alfons, Yang, Wei -Chang D., Zander, Ole, Stach, Eric A., Unold, Thomas, and Agrawal, Rakesh. 2015. "The role of interparticle heterogeneities in the selenization pathway of Cu-Zn-Sn-S nanoparticle thin films: A real-time study". United States. doi:10.1039/C5TC01139F. https://www.osti.gov/servlets/purl/1214519.
@article{osti_1214519,
title = {The role of interparticle heterogeneities in the selenization pathway of Cu-Zn-Sn-S nanoparticle thin films: A real-time study},
author = {Carter, Nathaniel J. and Mainz, Roland and Walker, Bryce C. and Hages, Charles J. and Just, Justus and Klaus, Manuela and Schmidt, Sebastian S. and Weber, Alfons and Yang, Wei -Chang D. and Zander, Ole and Stach, Eric A. and Unold, Thomas and Agrawal, Rakesh},
abstractNote = {Real-time energy dispersive x-ray diffraction (EDXRD) analysis has been utilized to observe the selenization of Cu-Zn-Sn-S nanoparticle films coated from three nanoparticle populations: Cu- and Sn-rich particles roughly 5 nm in size, Zn-rich nanoparticles ranging from 10 to 20 nm in diameter, and a mixture of both types of nanoparticles (roughly 1:1 by mass), which corresponds to a synthesis recipe yielding CZTSSe solar cells with reported total-area efficiencies as high as 7.9%. The EDXRD studies presented herein show that the formation of copper selenide intermediates during the selenization of mixed-particle films can be primarily attributed to the small, Cu- and Sn-rich particles. Moreover, the formation of these copper selenide phases represents the first stage of the CZTSSe grain growth mechanism. The large, Zn-rich particles subsequently contribute their composition to form micrometer-sized CZTSSe grains. In conclusion, these findings enable further development of a previously proposed selenization pathway to account for the roles of interparticle heterogeneities, which in turn provides a valuable guide for future optimization of processes to synthesize high quality CZTSSe absorber layers.},
doi = {10.1039/C5TC01139F},
journal = {Journal of Materials Chemistry. C},
number = 27,
volume = 3,
place = {United States},
year = {2015},
month = {6}
}