Spectroscopic Ellipsometry and Luminescence Properties of Low Temperature Sputter-Deposited Zinc Oxide Thin Films: Cryogenic Self-Stress-Induced Crystallization

Zinc oxide (ZnO) thin films were deposited by radio-frequency reactive magnetron sputtering at a cryogenic substrate temperature of −78 °C to explore a novel low-thermal-budget route for semiconductor growth. Despite the extremely low temperature, X-ray diffraction revealed spontaneous partial crystallization of wurtzite ZnO upon warming to room temperature, driven by strain relaxation and stress coupling at the ZnO/SiO2 interface. Atomic-force and scanning-electron microscopies confirmed nanoscale hillock and ridge morphologies that correlate with in-plane compressive stress and out-of-plane tensile strain. Spectroscopic ellipsometry, modeled using a general oscillator (GO) mathematical model approach, determined a film thickness of 60.81 nm, surface roughness of 3.75 nm, and a direct optical bandgap of 3.40 eV. Photoluminescence spectra exhibited strong near-band-edge emission modulated with LO-phonon replicas at 300 K, indicating robust exciton–phonon coupling. This study demonstrates that ZnO films grown at cryogenic conditions can undergo substrate-induced self-crystallize upon warming, which eliminates the need for thermal annealing. The introduced cryogenic self-crystallization regime offers a new pathway for depositing crystalline semiconductors on thermally sensitive or flexible substrates where heating is undesirable, enabling future optoelectronic and photonic device fabrication under ultra-low thermal-budget conditions.