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Issue 42, 2016
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Understanding the phase formation kinetics of nano-crystalline kesterite deposited on mesoscopic scaffolds via in situ multi-wavelength Raman-monitored annealing

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Abstract

Kesterite, a highly promising photo-absorbing crystalline form of Cu2ZnSnS4 (CZTS), has been prepared via various routes. However, the lack of in-depth understanding of the dynamic phase formation process of kesterite leads to difficulties in optimizing its annealing conditions, hence its light harvesting performance. In this paper, in situ Raman monitored-annealing is applied to study the phase formation kinetics of nano-crystalline kesterite from a precursor deposited on a TiO2 mesoscopic scaffold. By performing in situ Raman annealing under different experimental conditions and wavelengths, several facts have been discovered: kesterite crystallization starts at as low as 170 °C, but after short time annealing at 300 °C followed by cooling, the initially formed kesterite is found to decompose. Annealing at 400 °C or higher is proven to be sufficient for stabilizing the kesterite phase. Annealing at the higher temperature of 500 °C is necessary though to promote a complete reaction and thus eliminate the parasitic copper tin sulfide (CTS) impurity intermediates identified at lower annealing temperatures. More importantly, the real-time temperature dependence of Raman peak intensity enhancement, shift and broadening for CZTS is established experimentally at 500 °C for 1 h, providing a valuable reference in future CZTS research. This work demonstrates the significance of using in situ Raman spectroscopy in elucidating the kesterite phase formation kinetics, a critical step towards full crystal phase control − a prerequisite for developing fully functional CZTS-based optoelectronic devices.

Graphical abstract: Understanding the phase formation kinetics of nano-crystalline kesterite deposited on mesoscopic scaffolds via in situ multi-wavelength Raman-monitored annealing

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Publication details

The article was received on 19 Aug 2016, accepted on 30 Sep 2016 and first published on 30 Sep 2016


Article type: Paper
DOI: 10.1039/C6CP05759D
Citation: Phys. Chem. Chem. Phys., 2016,18, 29435-29446
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    Understanding the phase formation kinetics of nano-crystalline kesterite deposited on mesoscopic scaffolds via in situ multi-wavelength Raman-monitored annealing

    Z. Wang, S. Elouatik and G. P. Demopoulos, Phys. Chem. Chem. Phys., 2016, 18, 29435
    DOI: 10.1039/C6CP05759D

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