Search for: All records

Abstract Chalcogenide perovskites, particularly BaZrS₃, hold promise for optoelectronic devices owing to their exceptional light absorption and inherent stability. However, thin films obtained at lower processing temperatures typically result in small grain sizes and inferior transport properties. Here we introduce an approach employing co-sputtering elemental Ba and Zr targets followed by CS₂sulfurization, with a judiciously applied NaF capping layer. NaF acts as a flux agent during sulfurization, leading to marked increase in grain size and improved crystallinity. This process results in near-stoichiometric films with enhanced photoresponse. Terahertz spectroscopy further reveals a carrier mobility more than two orders of magnitude higher than those obtained from field-effect transistor measurements, suggesting that bulk transport is limited by grain boundary scattering. Our results demonstrate flux-assisted sulfurization as an effective strategy to improve the crystallinity of chalcogenide perovskite thin films for optoelectronic applications. Graphical abstract 

In this work, we demonstrate an ultrasensitive, visible-blind ultraviolet (UV) photodetector based on perovskite–polymer hybrid structure. A novel wide-band-gap vacancy-ordered lead-free inorganic perovskite Cs2SnCl6 with Nd3+ doping is employed in the active layer of this hybrid photodetector. Remarkably, with interfacial charge-controlled hole-injection operating mechanism, our device achieves a maximum detectivity of 6.3 × 1015 Jones at 372 nm, fast photoresponse speed with rise time and fall time in the order of milliseconds, and a large linear dynamic range of 118 dB. The performance is significantly better than most of the existing organic and inorganic semiconductor UV photodetectors reported so far, and its detectivity is close to 1 order of magnitude higher than that of the photomultiplication tube (PMT) in the UV region. In addition, the photodetector demonstrated excellent environmental stability, which is critical for commercial deployment of perovskite-based optoelectronic devices. The results presented in this work open a new route toward development of high-performance optoelectronic devices using perovskite-based hybrid nanomaterial systems. 

Ternary sulfides and selenides in the distorted-perovskite structure (“chalcogenide perovskites”) are predicted by theory to be semiconductors with a band gap in the visible-to-infrared and may be useful for optical, electronic, and energy conversion technologies. Here we use computational thermodynamics to predict the pressure–temperature phase diagrams for select chalcogenide perovskites. Our calculations incorporate formation energies calculated by density functional theory, and empirical estimates of heat capacities. We highlight the windows of thermodynamic equilibrium between solid chalcogenide perovskites and the vapor phase at high temperature and very low pressure. These results can guide the adsorption-limited growth of ternary chalcogenides by molecular beam epitaxy. 

Abstract Ternary sulfides and selenides in the distorted-perovskite structure (“chalcogenide perovskites”) are predicted by theory to be semiconductors with band gap in the visible-to-infrared and may be useful for optical, electronic, and energy conversion technologies. Density functional theory can be used in combination with computational thermodynamics to predict the pressure-temperature phase diagrams for chalcogenide perovskites. We report results using the Strongly Constrained and Appropriately Normed (SCAN) and the rVV10 density functionals, and compare to previously-published results using the PBEsol functional. We highlight the windows of thermodynamic equilibrium between solid chalcogenide perovskites and the vapor phase at high temperature and very low pressure. These phase diagrams can guide adsorption-limited growth of ternary chalcogenides by molecular beam epitaxy (MBE).