Highly Photosensitive Lead Sulfide Thin Films Grown by H₂S Free MOCVD Using a Single Source Metal‐Organic Precursor

Abstract High‐quality lead sulfide (PbS) films are deposited on selected substrate chemistries by an H₂S‐free metal‐organic chemical vapor deposition (MOCVD) process using a single‐source metal‐organic complex (Pb(dmampS)₂). The complex is synthesized via a salt metathesis reaction between PbCl₂ and lithium 1‐(dimethylamino)‐2‐methylpropane‐2‐thiolate (Li(dmampS)) in diethyl ether. Subsequent film deposition is conducted by a simple thermolysis process in the absence of H₂S, yet chemical and structural analysis confirm chemically stoichiometric and homogenous films. Mechanistic studies with electron impact mass spectroscopy (EIMS) and gas chromatography mass spectroscopy (GCMS) suggest the selective cleavage of C−S bonds in the complex as the reason for the facile PbS formation with negligible impurity incorporation. The high crystallinity, low hole concentrations, and charge transport properties comparable and in many cases superior to films produced by atomic layer deposition (ALD) testify to the quality of the films. Lastly, rigid and flexible photodetectors fabricated with the PbS films exhibit considerably high photocurrents, reliable switching characteristics, and high sensitivity over a broad spectral bandwidth, highlighting the potential for realizing practical broadband photodetectors.