The inorganic perovskite CsPbI3 is a promising material for optoelectronic applications like photodetectors and solar cells due to its suitable bandgap and excellent properties. In this work, nanostructured CsPbI3 thin films were deposited on glass and silicon substrates by pulsed laser deposition (PLD) at laser fluences ranging from 5.7 to 10 J/cm2. Systematic characterization revealed that increasing the laser fluence significantly enhances the crystallinity, phase purity, optical emission intensity, charge carrier concentration (up to 1.38 × 1012 cm−3), and mobility (up to 164.7 cm2/Vs) of the CsPbI3 films. An optimal laser fluence of 10 J/cm2 resulted in large, elongated grains over 280 nm, tightly packed films with minimal defects, and a suitable bandgap of 1.83 eV CsPbI3/Si heterojunction photodetectors were fabricated, with the device made at 8.5 J/cm2 exhibiting maximum responsivity of 8 A/W at 600 nm, detectivity exceeding 1014 Jones, external quantum efficiency up to 17.5 × 102 %, and a high ON/OFF ratio of 225 under illumination. The photodetector performance was strongly correlated with the optimized structural order, morphology, and optoelectronic quality achieved by careful control of the laser fluence during PLD. This work highlights PLD as an effective technique for realizing high-quality CsPbI3 films with tailored properties for advanced photodetection and photovoltaic applications.
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