Chemical Vapor Deposited Thin Palladium Sulfide Crystals for Highly Photoresponsive Photodetector

Nonlayered palladium sulfide (PdS) is of interest due to its rich physical properties and promising applications in optoelectronic devices. However, the growth of thin nonlayered PdS remains challenging because of its intrinsic 3D lattice structure. Here, the first demonstration of the direct synthesis of thin rectangular PdS ribbons/flakes on SiO2/Si substrates by a facile chemical vapor deposition (CVD) approach is presented. The atomic structure and high crystalline quality of CVD‐derived PdS crystals are shown by scanning transmission electron microscopy. The nonlinear saturable absorption and absorption enhancement are revealed by using ultrafast optical pump‐probe spectroscopy, and the photocarrier dynamics present the hot phonon bottleneck and Auger recombination effects. Additionally, the Raman vibration modes display the polarization‐dependent properties verified by angle‐resolved polarized Raman spectroscopy. Importantly, the photodetector based on PdS ribbon demonstrates a decent photoresponsivity of ≈7.7 × 103 A W−1. These results provide an effective way to form thin nonlayered PdS with potential applications in the field of photodetection. Thin nonlayered PdS crystals are synthesized on SiO2/Si substrates with a thickness down to 8.2 nm by a facile chemical vapor deposition strategy. The atomic structure and high crystalline quality of CVD‐derived PdS crystals are shown by scanning transmission electron microscopy. Significantly, the PdS‐based photodetector shows a high photoresponsivity of ≈7.7 × 103 A W−1 under 470 nm laser.