1：Experimental Design and Method Selection:

A Nd-YAG laser (third harmonic 355 nm,

2：7 ns) was used for ablation of Al-doped ZnO target. The deposition chamber was evacuated to a base pressure of 10?3 Pa, and then introduced with different background gas (O2 or He or Ar) to obtain a partial pressure (6 Pa–3 Pa) for deposition. Sample Selection and Data Sources:

Silicon (p-Si 100) and glass (Corning #26003) substrate were ultrasonically cleaned prior to use. They were placed

3：5 cm from the target. List of Experimental Equipment and Materials:

Nd-YAG laser (EKSPLA, NL301), Al-doped ZnO target (Kurt J. Lesker,

4：99% purity, 98% ZnO + 2wt% Al2O3), spectrometer (Ocean optics, S2000), atomic force microscopy (AFM) (Nanosurf), scanning electron microscope (SEM) (Hitachi, s1510, 15 kV), X-ray diffraction (XRD) (PANalytical, Empyrean). Experimental Procedures and Operational Workflow:

Deposition was carried out at room temperature for 45 min with at a repetition rate of 10 Hz. The laser beam was focused on the target at 45° with the dimension of ~1 mm x

5：8 mm. The laser fluence was kept at 2 J/cm2 for all deposition. Data Analysis Methods:

The plasma plume was measured by using time-integrated, optical emission spectroscopy and ion time of flight (TOF) measurements. The properties of the deposited ZnO thin films were characterized by UV–vis–NIR spectrophotometer, AFM, SEM, and XRD.