PbSe nanocrystal quantum dots (NQDs) are a promising active material for a range of optoelectronic devices, including solar cells, high-sensitivity infrared (IR) photodetectors, and IR-emitting diodes and lasers. However, device realization has been constrained by these NQDs' chemical instability toward oxidation, which leads to uncontrollable changes in optical and electronic properties. Here, we present a simple method to enhance the stability of PbSe NQDs against oxidation and to improve their optical properties through reaction with molecular chlorine. The chlorine molecules preferentially etch out surface Se ions and react with Pb ions to form a thin (1-2 monolayers) PbCl(x) passivation layer which effectively prevents oxidation during long-term air exposure while passivating surface trap states to increase photoluminescence efficiency and decrease photocharging. Our method is simple, widely applicable to PbSe and PbS NQDs of a range of sizes, compatible with solution-based processes for fabricating NQD-based devices, and effective both in solution and in solid NQD films; thus, it is a practical protocol for facilitating advances over the full range of optoelectronic applications.
Bromine and chlorine co-doped nanocrystalline titanium dioxide are synthesized by a hydrothermal method using titanium chloride in a mixed hydrobromic acid-ethanol system. TiO 2 with anatase, mixed anatase/rutile, rutile, mixed rutile/brookite, mixed anatase/rutile/ brookite, and rutile phases are obtained, in that order, by increasing the acidity through addition of HBr. Brand Clco-doping causes the absorption edge of TiO 2 to shift to a lower energy region. The photocatalytic activity of doped TiO 2 with mixed anatase/rutile phases exceeds that of commercial TiO 2 photocatalyst Degussa P-25 for water splitting into H 2 and O 2 under ultraviolet light.
A transparent stretchable conductor, in which well‐aligned CNT ribbons are embedded in poly(dimethylsiloxane) (PDMS) (CNT/PDMS film), is presented. Due to the good inter‐tube contact and stable CNT arrangement in the CNT ribbons, the CNT/PDMS film can maintain stable conductivity under repetitive stretching to strains up to 100%.
One process limiting the performance of solar cells is rapid cooling (thermalization) of hot carriers generated by higher-energy solar photons. In principle, the thermalization losses can be reduced by converting the kinetic energy of energetic carriers into additional electron-hole pairs via carrier multiplication (CM). While being inefficient in bulk semiconductors this process is enhanced in quantum dots, although not sufficiently high to considerably boost the power output of practical devices. Here we demonstrate that thick-shell PbSe/CdSe nanostructures can show almost a fourfold increase in the CM yield over conventional PbSe quantum dots, accompanied by a considerable reduction of the CM threshold. These structures enhance a valence-band CM channel due to effective capture of energetic holes into long-lived shell-localized states. The attainment of the regime of slowed cooling responsible for CM enhancement is indicated by the development of shell-related emission in the visible observed simultaneously with infrared emission from the core.
Separation of CO₂ and N₂ from CH₄ is significantly important in natural gas upgrading, and capture/removal of CO₂, CH₄ from air (N₂) is essential to greenhouse gas emission control. Adsorption equilibrium and kinetics of CO₂, CH₄, and N₂ on an ordered mesoporous carbon (OMC) sample were systematically investigated to evaluate its capability in the above two applications. The OMC was synthesized and characterized with TEM, TGA, small-angle XRD, and nitrogen adsorption/desorption measurements. Pure component adsorption isotherms of CO₂, CH₄, and N₂ were measured at 278, 298, and 318 K and pressures up to 100 kPa, and correlated with the Langmuir model. These data were used to estimate the separation selectivities for CO₂/CH₄, CH₄/N₂, and CO₂/N₂ binary mixtures at different compositions and pressures according to the ideal adsorbed solution theory (IAST) model. At 278 K and 100 kPa, the predicted selectivities for equimolar CO₂/CH₄, CH4/N₂, and CO₂/N₂ are 3.4, 3.7, and 12.8, respectively; and the adsorption capacities for CH₄ and CO₂ are 1.3 and 3.0 mmol/g, respectively. This is the first report of a versatile mesoporous material that displays both high selectivities and large adsorption capacities for separating CO₂/CH₄, CH₄/N₂, and CO₂/N₂ mixtures.
Two-dimensional organic–inorganic perovskites have attracted considerable interest recently. Here, we present a systematic study of the temperature-dependent photoluminescence on phase pure (n-BA)2(MA) n−1Pb n I3n+1 (n = 1–5) and (iso-BA)2(MA) n−1Pb n I3n+1 (n = 1–3) microplates obtained by mechanical exfoliation. The photoluminescence peak position gradually changes from a red-shift for n = 1 to a blue-shift for n = 5 with an increase in temperature in the (n-BA)2(MA) n−1Pb n I3n+1 (n = 1–5) series, while only a monotonous blue-shift has been observed for the (iso-BA)2(MA) n−1Pb n I3n+1 (n = 1–3) series, which can be attributed to the competition between the thermal expansion interaction and electron–phonon interaction. In the (n-BA)2(MA) n−1Pb n I3n+1 (n = 1–5) series, the thermal expansion interaction and electron–phonon interaction are both gradually enhanced and the former progressively dominates the latter from n = 1 to n = 5, resulting in the band gap versus temperature changing from a red-shift to a blue-shift. In contrast, both of these factors show a weaker layer thickness dependence, leading to the monotonous blue-shift in the (iso-BA)2(MA) n−1Pb n I3n+1 (n = 1–3) series.
The use of semiconductor nanocrystal quantum dots (QDs) in optoelectronic devices typically requires postsynthetic chemical surface treatments to enhance electronic coupling between QDs and allow for efficient charge transport in QD films. Despite their importance in solar cells and infrared (IR) light-emitting diodes and photodetectors, advances in these chemical treatments for lead chalcogenide (PbE; E = S, Se, Te) QDs have lagged behind those of, for instance, II-VI semiconductor QDs. Here, we introduce a method for fast and effective ligand exchange for PbE QDs in solution, resulting in QDs completely passivated by a wide range of small anionic ligands. Due to electrostatic stabilization, these QDs are readily dispersible in polar solvents, in which they form highly concentrated solutions that remain stable for months. QDs of all three Pb chalcogenides retain their photoluminescence, allowing for a detailed study of the effect of the surface ionic double layer on electronic passivation of QD surfaces, which we find can be explained using the hard/soft acid-base theory. Importantly, we prepare highly conductive films of PbS, PbSe, and PbTe QDs by directly casting from solution without further chemical treatment, as determined by field-effect transistor measurements. This method allows for precise control over the surface chemistry, and therefore the transport properties of deposited films. It also permits single-step deposition of films of unprecedented thickness via continuous processing techniques, as we demonstrate by preparing a dense, smooth, 5.3-μm-thick PbSe QD film via doctor-blading. As such, it offers important advantages over laborious layer-by-layer methods for solar cells and photodetectors, while opening the door to new possibilities in ionizing-radiation detectors.
Epitaxial c-axis oriented BiFeO3 (BFO) thin films were deposited on (001) Nb-doped SrTiO3 (Nb-STO) substrates by pulsed laser deposition. Introducing Bi vacancies caused the BFO thin film to evolve to a p-type semiconductor and formed a p-n heterojunction with an n-type semiconductor Nb-STO. The current density versus voltage (J-V) and capacitance versus voltage (C-V) characteristics of the heterojunction were investigated. A typical rectifying J-V effect was observed with a large rectifying ratio of 5×104. Reverse C-V characteristics exhibited a linear 1∕C2 versus V plot, from which a built-in potential of 0.6V was deduced. The results show a potential application of BFO/Nb-STO heterojunction for oxide electronics.
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