Improved Heterojunction Quality in Cu2O-based Solar Cells Through the Optimization of Atmospheric Pressure Spatial Atomic Layer Deposited Zn1-xMgxO

Atmospheric pressure spatial atomic layer deposition (AP-SALD) was used to deposit n-type ZnO and Zn_1-xMg_xO thin films onto p-type thermally oxidized Cu₂O substrates outside vacuum at low temperature. The performance of photovoltaic devices featuring atmospherically fabricated ZnO/Cu₂O heterojunction was dependent on the conditions of AP-SALD film deposition, namely, the substrate temperature and deposition time, as well as on the Cu₂O substrate exposure to oxidizing agents prior to and during the ZnO deposition. Superficial Cu₂O to CuO oxidation was identified as a limiting factor to heterojunction quality due to recombination at the ZnO/Cu₂O interface. Optimization of AP-SALD conditions as well as keeping Cu₂O away from air and moisture in order to minimize Cu₂O surface oxidation led to improved device performance. A three-fold increase in the open-circuit voltage (up to 0.65 V) and a two-fold increase in the short-circuit current density produced solar cells with a record 2.2% power conversion efficiency (PCE). This PCE is the highest reported for a Zn_1-xMg_xO/Cu₂O heterojunction formed outside vacuum, which highlights atmospheric pressure spatial ALD as a promising technique for inexpensive and scalable fabrication of Cu₂O-based photovoltaics.