Towards the growth of Cu2ZnSn1 xGexS4 thin films by a single-stage process: Effect of substrate temperature and composition

9 págs.; 7 figs.; 2 tabs.Cu2ZnSn1-xGexS4 (CZTGS) thin films prepared by flash evaporation of a Zn-rich Cu2ZnSn0.5Ge0.5S4 bulk compound in powder form, and a subsequent thermal annealing in S containing Ar atmosphere are studied. The effect of the substrate temperature during evaporation and the initial composition of the precursor powder on the growth mechanism and properties of the final CZTGS thin film are investigated. The microstructure of the films and elemental depth profiles depend strongly on the growth conditions used. Incorporation of Ge into the Cu2ZnSnS4 lattice is demonstrated by the shift of the relevant X-ray diffraction peaks and Raman vibrational modes towards higher diffraction angles and frequencies respectively. A Raman mode at around 348-351 cm-1 is identified as characteristic of CZTGS alloys for x = [Ge]/([Sn]+[Ge]) = 0.14-0.30. The supply of Ge enables the reduction of the Sn loss via a saccrifical Ge loss. This fact allows increasing the substrate temperature up to 350º C during the evaporation, forming a high quality kesterite material and therefore, reducing the deposition process to one single stage & 2015 Elsevier B.V. All rights reserved.RC acknowledges financial support from Spanish MINECO within the Ramón y Cajal programme (RYC-2011-08521) and VIR for the Juan de la Cierva fellowship (JCI-2011-10782). GB also acknowledges the CSIC-JAE Pre-doctoral Program, co-funded by the European Social Fund. This work was supported by the Marie Curie-IRSES Project (PVICOKEST, GA: 269167), Marie Curie-ITN project (KESTCELL, GA: 316488), DAAD project (INTERKEST, Ref: 57050358), and MINECO projects (SUNBEAM, ENE2013-49136-C4-3-R) (TEC2012- 38901-C02-01). A. Scheu is acknowledged for GDOES measurements.Peer Reviewe