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In this paper, we report passivation properties of inverted pyramidal nanostructure based multi-crystalline silicon (mc-Si) by Al
2
O
3
films with spin-coating method. Precursors AlCl
3
and Al(acac)
3
for Al
2
O
3
films were chosen for comparison. Al
2
O
3
/SiO
x
stacks were found to be able to passivate the nanostructured surface well. With the number of spin-coating up to five, the Al
2
O
3
films could conformally attach the nanostructure. The weighted average reflectance values (ranging from 400–900 nm) of the passivated silicon surface could be reduced to 10.74% (AlCl
3
) and 11.12% (Al(acac)
3
), and the effective carrier lifetime could reach 7.84 and 16.98 μs, respectively. This work presented a potential process to fabricate low cost high efficiency mc-Si solar cells.