Infrared solar cells that utilize low-bandgap colloidal quantum dots (QDs) are promising devices to enhance the utilization of solar energy by expanding the harvested photons of common photovoltaics into the infrared region. However, the present technology for synthesis of PbS QDs cannot produce highly efficient infrared solar cells. Here, we develop a general synthesis framework for low-bandgap PbS QDs (0.65-1 eV) via cation-exchange from ZnS nanorods (NRs). First, ZnS NRs are converted to superlattices with segregated PbS domains within each rod. Then, sulfur precursors are released via dissolution of the ZnS NRs during the cation-exchange, which promotes size-focusing of PbS QDs. PbS QDs synthesized through this new method have the advantages of high monodispersity, ease of size control, in-situ passivation of chloride, high stability, and "clean" surface. We fabricated infrared solar cells based on these PbS QDs with different bandgaps, using conventional ligand exchange and device structure. All of our devices produced in this manner show excellent performance, showcasing the high quality of our PbS QDs. The highest performance of infrared solar cells was achieved using ~0.95 eV PbS QDs, exhibiting an efficiency of 10.0% under AM 1.5 solar illumination, a perovskitefiltered efficiency of 4.2% and a silicon-filtered efficiency of 1.1%.
Trap states in colloidal quantum dot (QD) solids significantly affect the performance of QD solar cells, because they limit the open-circuit voltage and short circuit current. The {100} facets of PbS QDs are important origins of trap states due to their weak or missing passivation. However, previous investigations focused on synthesis, ligand exchange, or passivation approaches and ignored the control of {100} facets for a given dot size. Herein, trap states are suppressed from the source via facet control of PbS QDs. The {100} facets of ≈3 nm PbS QDs are minimized by tuning the balance between the growth kinetics and thermodynamics in the synthesis. The PbS QDs synthesized at a relatively low temperature with a high oversaturation follow a kinetics-dominated growth, producing nearly octahedral nanoparticles terminated mostly by {111} facets. In contrast, the PbS QDs synthesized at a relatively high temperature follow a thermodynamics-dominated growth. Thus, a spherical shape is preferred, producing truncated octahedral nanoparticles with more {100} facets. Compared to PbS QDs from thermodynamics-dominated growth, the PbS QDs with less {100} facets show fewer trap states in the QD solids, leading to a better photovoltaic device performance with a power conversion efficiency of 11.5%.
The interaction between residual stress and fatigue crack growth rate has been investigated in middle tension and compact tension specimens machined from a variable polarity plasma arc welded aluminium alloy 2024-T3 plate. The specimens were tested at three levels of applied constant stress intensity factor range. Crack closure was continuously monitored using an eddy current transducer and the residual stresses were measured with neutron diffraction. The effect of the residual stresses on the fatigue crack behaviour was modelled for both specimen geometries using two approaches: a crack closure approach where the effective stress intensity factor was computed; and a residual stress approach where the effect of the residual stresses on the stress ratio was considered. Good correlation between the experimental results and the predictions were found for the effective stress intensity factor approach at a high stress intensity factor range whereas the residual stress approach yielded good predictions at low and moderate stress intensity factor ranges. In particular, the residual stresses accelerated the fatigue crack growth rate in the middle tension specimen whereas they decelerated the growth rate in the compact tension sample, demonstrating the importance of accurately evaluating the residual stresses in welded specimens which will be used to produce damage tolerance design data.
2D halide semiconductors, a new family of 2D materials in addition to transition metal dichalcogenides, present ultralow dark current and high light conversion yield, which hold great potential in photoconductive detectors. Herein, a facile aqueous solution method is developed for the preparation of large-scale 2D lead dihalide nanosheets (PbF I ). High-performance UV photodetectors are successfully implemented based on 2D PbF I nanosheets. By modulating the components of halogens, the bandgap of PbF I nanosheets can be tuned to meet varied detection spectra. The photoresponse dependence on incident power density, wavelength, detection environment, and temperature are systematically studied to investigate their detection mechanism. For PbI photodetectors, they are dominantly driven by a photoconduction mechanism and show a fast response speed and a low noise current density. A high normalized detectivity of 1.5 × 10 Jones and an I /I ratio up to 10 are reached. On the other hand, PbFI photodetectors demonstrate a photogating mechanism mediated by trap states showing high responsivity. The novel 2D halide materials with wide bandgaps, superior detection performance, and facile synthesis process can enrich the Van der Waals solids family and hold great potential for a wide variety of applications in advanced optoelectronics.
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