Guided by predictive discovery framework, we investigate bismuth triiodide (BiI3) as a candidate thin-film photovoltaic (PV) absorber. BiI3 was chosen for its optical properties and the potential for "defect-tolerant" charge transport properties, which we test experimentally by measuring optical absorption and recombination lifetimes. We synthesize phase-pure BiI3 thin films by physical vapor transport and solution processing and single-crystals by an electrodynamic gradient vertical Bridgman method. The bandgap of these materials is ∼1.8 eV, and they demonstrate room-temperature band-edge photoluminescence. We measure monoexponential recombination lifetimes in the range of 180-240 ps for thin films, and longer, multiexponential dynamics for single crystals, with time constants up to 1.3 to 1.5 ns. We discuss the outstanding challenges to developing BiI3 PVs, including mechanical and electrical properties, which can also inform future selection of candidate PV absorbers.
As the field of flash sintering expands, more diverse flash processes are emerging that exhibit complex mechanisms and kinetics. Reactive flash sintering studies have been performed using precursor oxides and have yet to explore redox reactions. We show that Mn2O3 transforms into Mn3O4 during stage III of flash sintering via a moving reaction front, propagating from an electrode if sufficient energy is supplied. The power density and sample temperature increases as the transformation progresses due to the lower resistivity of Mn2O3 vs Mn3O4, a secondary thermal runaway effect, further confirming the presence of a transformation front. Additionally, in many studies, the contact resistance is accounted for, but not utilized. The energy for the transformation may either be supplied by the contact resistance–induced Joule heating or the furnace. Room‐temperature impedance measurements demonstrate that Pt electrodes provide substantial contact resistance while Ag electrodes do not. The impedance study demonstrates that it is critical to select the appropriate electrode material to maximize or minimize contact resistance. The contact resistance may be used to create a hot spot and propagate a transformation front in any endothermic reduction reaction that occurs below 950°C in electronic conductors.
The oxalate route offers a controlled approach to synthesize pure Ba 1-x Sr x TiO 3 (BST) (0 ≤ x ≤ 1) nanoparticles (≈ 150 nm in diameter). Reduced BST dense nanoceramics were obtained by spark plasma sintering (SPS) and then annealed for a short time to reach colossal permittivity (′ r = 10 5) with low dielectric losses (tan ı = 0.03) at 1 kHz and 300 K. The effects of Ba-Sr substitution on structural, microstructural and electrical properties were analyzed. Comprehensive analysis of the electrical properties indicates that polaron hopping, mediated by Ti 3+ ions and oxygen vacancies is the main contributing mechanism to colossal permittivity in Ba-rich BST compounds. Substitution of Ba by Sr reduced the contribution of polaron hopping and led to a decrease of real and imaginary parts of permittivity, while preserving interfacial polarization and yielding better temperature stability. The lowest temperature coefficient of capacitance, or TCC (variation of capacitance between 310 K and 450 K) value, i.e., 44 ppm K −1 , is obtained for SrTiO 3 .
Reactive flash sintering has been demonstrated as a method to rapidly densify and synthesize ceramic materials, but determining the extent of chemical reactions can be complex since the maximum temperature reached by the sample may be brief in time. The black body radiation (BBR) model has been shown to accurately predict the sample temperature during the steady state of flash (stage III). This work demonstrates situations where the BBR model alone does not accurately predict when a phase transformation will occur. We examine the model reactions of CuO reduction to Cu 2 O during stage II and Mn 2 O 3 reduction to Mn 3 O 4 in stage III. In CuO, highly resistive samples result in initially localized current flow, a stochastic process resulting in inhomogeneous heating and error in the BBR model during stage II. CuO reduction does not occur in constant heating rate experiments with 6.25 V/mm fields, even though the sample temperature momentarily exceeds the phase transformation temperature. Increased furnace heating to 950°C before application of a field is required to drive the transition. In Mn 2 O 3 , the calculated sample temperature of the gauge is less than the transformation temperature, but localized heating at the contact will exceed the transformation temperature, causing the transformation to propagate away from the electrode during stage III. This work demonstrates two forms of inhomogeneity (local, stochastic current flow, and local contact resistance) that result in a complex thermal profile of the sample. This profile should be interrogated to understand reaction kinetics, and can be beneficial when engineered.
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