Abstract
We present a comprehensive ultrafast spectroscopy-based study on the delocalization of doping-induced carriers in Si nanocrystals (NCs). To this end we prepare thin films of differently sized doped Si NCs and vary the doping configurations from singly P and B doping to simultaneously P and B co-doping. We show that the NC size orchestrates the level of delocalization of the doping-induced carriers. This can be understood in light of (1) the quantum confinement effect and (2) unscreened Coulomb interactions by moving further into the nanoscale. Both contributions affect the activation energy (ΔE) that is required to create free majority carriers. By varying the NC size in combination with the doping configuration we tune ΔE and control the delocalization of the doping-induced carriers. Most importantly, we show that there is a critical NC diameter of Dcritical ≈ 6 nm that describes the transition from a localized to a free carrier regime. In particular, our results show that optical bandgaps of ∼0.95 eV (optimal for carrier multiplication-facilitated solar cell power conversion) can be achieved in P–B co-doped Si NCs with DNC < Dcritical. These results indicate that the practical photovoltaic feasibility of co-doped Si NCs is not limited by the presence of some remaining free carriers in uncompensated NCs.
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