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The efficiency of nanoparticle (NP) solar cells has grown impressively in recent years, exceeding 16%. However, the carrier mobility in NP solar cells, and in other optoelectronic applications remains low, thus critically limiting their performance. Therefore, carrier transport in NP solids needs to be better understood to further improve the overall efficiency of NP solar cell technology. However, it is technically challenging to simulate experimental scale samples, as physical processes from atomic to mesoscopic scales all crucially impact transport. To rise to this challenge, here we report the development of TRIDENS: the  Tr ansport  i n  De fected  N anoparticle  S olids Simulator, that adds three more hierarchical layers to our previously developed HINTS code for nanoparticle solar cells. In TRIDENS, we first introduced planar defects, such as twin planes and grain boundaries into individual NP SLs superlattices (SLs) that comprised the order of 10 3  NPs. Then we used HINTS to simulate the transport across tens of thousands of defected NP SLs, and constructed the distribution of the NP SL mobilities with planar defects. Second, the defected NP SLs were assembled into a resistor network with more than 10 4  NP SLs, thus representing about 10 7  individual NPs. Finally, the TRIDENS results were analyzed by finite size scaling to explore whether the percolation transition, separating the phase where the low mobility defected NP SLs percolate, from the phase where the high mobility undefected NP SLs percolate drives a low-mobility-to-highmobility transport crossover that can be extrapolated to genuinely macroscopic length scales. For the theoretical description, we adapted the Efros-Shklovskii bimodal mobility distribution percolation model. We demonstrated that the ES bimodal theory’s two-variable scaling function is an effective tool to quantitatively characterize this low-mobility-to-high-mobility transport crossover.

Hierarchical carrier transport simulator for defected nanoparticle solids