Thin semiconductor CuInSe 2 and CuInS 2 films (CIS) with bandgap values (E g ) of around 1.04 eV (for selenide) and 1.5 eV (for sulfide) represent an important class of the currently developed light absorbers for solar energy harvesting. [1,2] Conversion efficiencies of 12±13 % were achieved on large area modules, [1] whereas close to 18 % was achieved with laboratory cells, [3] indicating a large potential for CIS-derived photovoltaic materials. For their preparation, a broad range of physical [1±3] and electrochemical deposition routes [4] are available. Typically, CIS films are created via a rapid thermal sintering of elemental Cu, In and Se layers evaporated on Mo-coated glass substrates. The photovoltaic cell is then completed by overcoating the CIS-macrograins with a thin CdS buffer layer and a metal± organic chemical vapor deposition derived, transparent Al/ ZnO window electrode. In this contribution, we address a low cost colloidal route to nanocrystalline ZnO/CIS bilayers on indium tin oxide (ITO) glass. For the film deposition, concentrated coating colloids, with size-quantized CuInS 2 particles were developed. It is well-established that size quantization in semiconductors (i.e. increasing bandgap energy with decreasing semiconductor dimension) takes place at particle dimensions smaller than the Wannier±Mott (WM) exciton of the corresponding macroscopic bulk phase.[5] By knowledge of the high frequency dielectric constant, e ¥ , and the reduced effective exciton mass, m = 1/(m ±1 e + m ±1 h ), one can calculate the WM-exciton Bohr radius according to R B = (e ¥ /m)´a B , with a B being the Bohr radius of the hydrogen atom. Taking the CIS bulk values [6] of e ¥ = 11, m e = 0.16 and m h = 1.3, we calculated the WM-exciton size to be 8.1 nm, which predicts a blue shift in the optical absorption threshold (below 826 nm = 1240/1.5 eV) for CIS-particle sizes below 8 nm. Figure 1 shows changes in the optical absorption spectrum during the CIS condensation. Condensation was induced on addition of bis(trimethylsilyl)sulfide to a mixture of Cu(I)±P(OPh) 3 and In(III)±P(OPh) 3 complexes (Cu/ In = 1) in Ar saturated acetonitrile (for details see Experimental).At sulfide concentrations~25 % (with respect to the present metals), the absorption spectrum exhibits a shoulder located at 370 nm that is strongly blue-shifted with respect to the bulk crystals (a gap energy difference of more than 2 eV). On further addition of the sulfide source (50 %), the absorption shoulder shifts from 370 nm to 400 nm, and the optical density rises due to increasing particle concentration. Under stoichiometric conditions (100 % S corresponds to the Cu:In:S stoichiometry of 1:1:2), a steep tail is observed with the absorption onset located near 580 nm.A remarkable dynamic color change accompanies this condensation process which can be seen with the naked eye. On each dropwise addition of the sulfide source, the color of the reacting solution rapidly changes from colorless to yellow to orange to red and becomes colorless or yellow agai...
Polycrystalline silicon (poly-Si) thin films have been prepared by electron-beam evaporation and thermal annealing for the development of thin-film solar cells on glass coated with ZnO:Al as a transparent, conductive layer. The poly-Si microstructure and photovoltaic performance were investigated as functions of the deposition temperature by Raman spectroscopy, scanning and transmission electron microscopies including defect analysis, x-ray diffraction, external quantum efficiency, and open circuit measurements. It is found that two temperature regimes can be distinguished: Poly-Si films fabricated by deposition at low temperatures (Tdep<400 °C) and a subsequent thermal solid phase crystallization step exhibit 1–3 μm large, randomly oriented grains, but a quite poor photovoltaic performance. However, silicon films deposited at higher temperatures (Tdep>400 °C) directly in crystalline phase reveal columnar, up to 300 nm big crystals with a strong ⟨110⟩ orientation and much better solar cell parameters. It can be concluded from the results that the electrical quality of the material, reflected by the open circuit voltage of the solar cell, only marginally depends on crystal size and shape but rather on the intragrain properties of the material. The carrier collection, described by the short circuit current of the cell, seems to be positively influenced by preferential ⟨110⟩ orientation of the grains. The correlation between experimental, microstructural, and photovoltaic parameters will be discussed in detail.
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