Paulauskas, Tadas | Engineering Papers

DOE OSTI2021

Computational design of passivants for CdTe grain boundaries

CdTe is the second most-widely deployed photovoltaic (PV) material due to its high efficiency and low manufacturing costs. Currently, polycrystalline CdTe (poly-CdTe) has a record efficiency of similar to 22%, which is still well below the theoretical limit (similar to 30%). Polycrystalline CdTe films that have incorporated Cl or Se show higher efficiency, possibly due to the segregation of these ions to the grain boundaries (GBs), where they may passivate the dangling bonds. However, the efficiency enhancement mechanisms of passivants in CdTe GBs, and the feasibility of employing alternative passivants, have not been well explored. Here, we present a systematic computational study of CdTe GBs with potential passivants, namely S, P, As, Se, and Sb on Te sites, and Na, Mg, Al, Sc, Cu, and Zn on Cd sites. Density functional theory (DFT) calculations were performed on GB dislocation core structures derived from scanning transmission electron microscopy (STEM) images of a model GB (bicrystal). We computed the segregation thermodynamics, electronic density of states, and charge variations near doped CdTe GBs. We find that segregation of impurities to GBs is thermodynamically favorable. For a Te-terminated core, Se, S, and P on Te sites effectively reduce midgap states. For both Cd-and Te-terminated dislocation cores, Sc and Al reduce midgap states when substituted for Cd atoms. Overall, the greatest improvement was achieved with co-doping, i.e. simultaneously substituting Te with Se and substituting Cd with Cu or Al. The elimination of midgap states is predicted to increase the photovoltaic efficiency of CdTe by reducing the recombination at grain boundaries.

14 SOLAR ENERGY↗

DOE OSTI2019

STEM characterization of solar cells

Photovoltaic (PV) devices consisting of a thin-film CdTe absorber layer on glass support have long been considered one of the leading technologies for reaching the Department of Energy’s 2030 cost target of less than 0.03/kWh. Here, the currently used device architectures include a thin transparent conductive oxide (TCO) on top of the glass superstrate following by very thin (<100 nm) polycrystalline emitter layer, typically CdS or more recently MgZnO (MZO). The CdTe absorber layer is usually up to 4 µm thick and polycrystalline, followed by the back contact (Figure 1). Typical CdTe thin-film layers are formed from rapid deposition techniques, such as close-spaced sublimation (CSS) or high-rate vapor-transport deposition (HRVDT). Both processes result in a polycrystalline CdTe photo-absorbing film, and such devices can be manufactured cheaply and efficiently at large scale. Record cell efficiencies as high as 22.1% have been demonstrated. However, such cell performances are still far from the theoretical limits (~30% for CdTe), and improvements have mostly been due to better light collection, rather than improvements in absorber conversion efficiency. The remaining obstacles to further improving these devices toward their theoretical limits concern improvements in the fill factor (FF) and, more importantly, open-circuit voltage (V oc ), which is still far from its limit. In fact, it is widely accepted that V oc is the limiting factor since it reaches only about 60% of the CdTe bandgap. This is in contrast to GaAs solar cells, which have reached a V oc of 80% of the bandgap. The reasons for this discrepancy have been identified as the low p -type doping concentrations of CdTe due to the formation of compensating defect states, a poor p-n junction, and the need for better backside ohmic contacts. High interfacial defect density at grain boundaries (GBs) and intragrain dislocations is also one of the main concerns because they contribute to the dark current. This is supported by the study of single-crystal-based CdTe solar cells that were able to reach Voc in excess of 1 V.

14 SOLAR ENERGY↗