Various quaternary ( ) chalcopyrite nanoparticles have been prepared from molecular single-source precursors via microwave decomposition. We were able to control the nanoparticle size, phase, stoichiometry, and solubility. Depending on the choice of surface modifiers used, we were able to tune the solubility of the resulting nanoparticles. This method has been used to generate up to 5？g of nanoparticles and up to 150？g from multiple batch reactions with excellent reproducibility. Data from UV-Vis, photoluminescence, X-ray diffraction, TEM, DSC/TGA-MS, and ICP-OES analyses have shown high reproducibility in nanoparticle size, composition, and bandgap. 1. Introduction For nearly three decades, chalcopyrite CuIn0.7Ga0.3Se2 (CIGS) and related materials have attracted much interest due to their potential applications in photovoltaic and other optoelectric devices [1–5]. Many thin film PV devices of CIGS set respectable power conversion efficiency of about 20% [6, 7]. In recent years, there have been increasing reports on using colloidal I–III–VI nanoparticle suspensions, composites, and inks to prepare PV devices. Solution processing strategies such as spin coating [8–10] and ink printing [1, 2, 4] are being explored for large areas of CIGS while lowering the overall costs. One of the key stoichiometric requirements is to consistently maintain In/Ga ratio to 0.7/0.3 from batch to batch. Previously, we reported the efficient syntheses of quaternary chalcopyrite nanoparticles with precise stoichiometric control by decomposition of a mixture of two I–III bimetallic single-source precursors (SSPs), (Ph3P)2Cu(μ-SEt)2In(SEt)2 (1), and (Ph3P)2Cu(μ-SEt)2Ga(SEt)2 (2), in the presence of 1,2-ethanedithiol via microwave irradiation [11]. Use of SSPs in preparation of nanomaterials presents distinct advantages such as precise control of reaction conditions and stoichiometry as SSPs contain all necessary elements in a single molecule. Despite the obvious advantages of SSPs, to our knowledge, no studies have been conducted using combinations of SSPs to form soluble and insoluble ternary and quaternary chalcopyrite nanoparticles. Microwave-assisted preparation of nanoparticles from SSPs offers advantages over traditional thermolysis as microwave provides rapid heating as well as greater homogeneity in the overall reaction temperature [12]. This usually allows for the preparation of nanoparticles with increased size control [13], dramatic decreases in reaction times, improved product purities, and reactions exhibiting good reproducibility and high yields [14, 15]. In our
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