Low‐Temperature Synthesis of Stable CaZn<sub>2</sub>P<sub>2</sub> Zintl Phosphide Thin Films as Candidate Top Absorbers
Shaham Quadir, Zhenkun Yuan, Guillermo L. Esparza, Sita Dugu, John S. Mangum, Andrew Pike, Muhammad Rubaiat Hasan, Gideon Kassa, Xiaoxin Wang, Yagmur Coban, Jifeng Liu, Kirill Kovnir, David P. Fenning, Obadiah G. Reid, Andriy Zakutayev, Geoffroy Hautier, Sage R. Bauers
Abstract
Abstract The development of tandem photovoltaics and photoelectrochemical solar cells requires new absorber materials with bandgaps in the range of ≈1.5–2.3 eV, for use in the top cell paired with a narrower‐gap bottom cell. An outstanding challenge is finding materials with suitable optoelectronic and defect properties, good operational stability, and synthesis conditions that preserve underlying device layers. This study demonstrates the Zintl phosphide compound CaZn 2 P 2 as a compelling candidate semiconductor for these applications. Phase‐pure, ≈500 nm‐thick CaZn 2 P 2 thin films are prepared using a scalable reactive sputter deposition process at growth temperatures as low as 100 °C, which is desirable for device integration. Ultraviolet‐visible spectroscopy shows that CaZn 2 P 2 films exhibit an optical absorptivity of ≈10 4 cm −1 at ≈1.95 eV direct bandgap. Room‐temperature photoluminescence (PL) measurements show near‐band‐edge optical emission, and time‐resolved microwave conductivity (TRMC) measurements indicate a photoexcited carrier lifetime of ≈30 ns. CaZn 2 P 2 is highly stable in both ambient conditions and moisture, as evidenced by PL and TRMC measurements. Experimental data are supported by first‐principles calculations, which indicate the absence of low‐formation‐energy, deep intrinsic defects. Overall, this study shall motivate future work integrating this potential top cell absorber material into tandem solar cells.