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The three A symmetry Raman modes of kesterite in Cu2ZnSnSe4

Rabie Djemour, Alex Redinger, Marina Mousel, Levent Gütay, Xavier Fontané, Victor Izquierdo-Roca, Alejandro Pérez-Rodríguez, and Susanne Siebentritt

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Abstract

We investigate CZTSe films by polarization dependent Raman spectroscopy. The main peaks at 170 cm−1, and 195 cm−1 are found to have A symmetry. The Raman signal at 170 cm−1 is found to be composed of two modes at 168 cm−1 and 172 cm−1. We attribute these three Raman peaks to the three A symmetry modes predicted for kesterite ordered Cu2ZnSnSe4. The main Raman peak is asymmetrically broadened towards lower energies. Possible sources of the broadening are tested through temperature and depth dependent measurements. The broadening is attributed to phonon confinement effects related to the presence of lattice defects.

©2013 Optical Society of America

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Figures (5)
Fig. 1
Fig. 1 Raman spectra from CZTSe absorber taken under parallel (black) and perpendicular (red) polarization configurations. Inset shows normalized spectra in the energy range 150-180cm−1.

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Fig. 2
Fig. 2 Micro Raman spectrum of CZTSe absorber restricted to the spectral area of 145-220 cm−1 (black). The main mode at 195cm−1 is fitted with two lorentzians(a)) or an asymmetrically broadened lorentzian(b)) (blue). The residual is plotted red. The other modes at 168, 172 cm−1 are fitted with two lorentzians (grey line).The green line shows the sum of the fits.

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Fig. 3
Fig. 3 Raman spectrum of CZTSe absorber restricted to the spectral area of 140-280 cm−1. The main mode is fitted with an asymmetrically broadened Lorentzian peak shape. The thin lines show the fit (blue) and residuals (red) of the data excluding the low intensity CZTSe peaks marked in grey, thick lines show fits and residuals with the low energy shoulder of the main mode (marked in blue) discarded when fitting.

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Fig. 4
Fig. 4 Normalized straight line background corrected micro Raman spectra of CZTSe absorber restricted to the spectral area of 150-220 cm−1. Both measurements were taken at the same spot at different excitation laser powers (black curve: 0.5 mW/micro spot; red curve: 2.5 mW/micro spot). Inset shows data prior to background subtraction.

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Fig. 5
Fig. 5 Two micro Raman spectra of CZTSe absorber restricted to the spectral area of 150-220 cm−1. Both measurements were taken at the same spot at different temperatures (black curve: 300 K; blue curve: 10 K).

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Tables (1)

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Table 1 Summary of DFT and experimentally acquired Raman active A symmetry mode energies (in cm−1) for CZTSe

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Equations (1)

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I( ω )=   I 0 ( 1+4 ( ωx F ) 2 ) ωx= ω− ω 0 1−α( ω− ω 0 F )
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