Optical absorbance was measured with an Agilent Cary 5000 spectrometer, and Flog-3 (HORIBA) was used to characterize the film PL, PL QY, and PL excitation spectra. The PL decay experiments were performed on the same samples using the same Fluorolog with a pulsed source at 408 nm (HORIBA NanoLED 405-LH), and the signal was recorded using Time-Correlated Single Photon Counting (TCSPC). TA was measured using a HELIOS femtosecond transient absorption spectrometer (Ultrafast Systems LLC) with a 450-nm laser (140 mJ cm−2). In situ fluorescence spectra were recorded using a USB2000+ spectrometer (Ocean Optics) with a 200-mm optical fiber in a N2-filled glovebox, and the excited light was at 390 nm from a UV lamp. The atomic force microscopy (AFM) surface morphology of the films was measured using the Bruker AFM system (FastSCAN). The ZnO nanoparticles were characterized using a JEOL-2100Plus transmission electron microscope with a 120-keV electron beam energy. The XRD characterizations were taken on a Bruker D8 system using Cu Kα (λ = 1.5405 Å) as the x-ray source and x-ray generator settings at 40 kV and 30 mA, respectively. X-ray photoemission spectroscopy (XPS) and UPS data were conducted using an ESCALAB 250Xi (Thermo Fisher Scientific). A monochromatic Al Kα line (1486.6 eV) was used for XPS, and He-I radiation (21.22 eV) with an applied bias of −10 V was used for UPS.

GIWAXS studies were performed at the BL16B1 beamline of Shanghai Synchrotron Radiation Facility, Shanghai, China using a beam energy of 10 keV (λ = 1.2398 Å) and a Mar 225 detector. Images were acquired with a 50-s (for 33, 50, and 100% samples) or 100-s (for FAI additive samples) exposure time. The distance between the sample and detector was 220 mm. The grazing incidence angles for all films were 0.1°, 0.2°, 0.5°, 1°, and 2°, respectively. The GIXSGUI (MATLAB toolbox) was used to analyze the raw patterns (42).

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