We have determined the Auger recombination kinetics of electrons and holes in colloidal CdSe-only and CdSe/CdS/ZnS core/shell nanoplatelets by time-resolved photoluminescence measurements. Excitation densities as high as an average of 18 electron−hole pairs per nanoplatelet were reached. Auger recombination can be described by second-order kinetics. From this we infer that the majority of electrons and holes are bound in the form of neutral excitons, while the fraction of free charges is much smaller. The biexciton Auger recombination rate in nanoplatelets is more than 1 order of magnitude smaller than for quantum dots and nanorods of equal volume. The latter is of advantage for application in lasers, light-emitting diodes, and photovoltaics.
We
show that intercalation of cations (Na+, Ca2+, Ni2+, and Co2+) into the interlayer region
of 1T-MoS2 is an effective strategy to lower the overpotential
for the hydrogen evolution reaction (HER). In acidic media the onset
potential for 1T-MoS2 with intercalated ions is lowered
by ∼60 mV relative to that for pristine 1T-MoS2 (onset
of ∼180 mV). Density functional theory (DFT) calculations show
a lowering in the Gibbs free energy for H-adsorption (ΔG
H) on these intercalated structures relative
to intercalant-free 1T-MoS2. The DFT calculations suggest
that Na+ intercalation results in a ΔG
H close to zero. Consistent with calculation, experiments
show that the intercalation of Na+ ions into the interlayer
region of 1T-MoS2 results in the lowest overpotential for
the HER.
Charge trapping is an ubiquitous process in colloidal quantum-dot solids and a major limitation to the efficiency of quantum dot based devices such as solar cells, LEDs, and thermoelectrics. Although empirical approaches led to a reduction of trapping and thereby efficiency enhancements, the exact chemical nature of the trapping mechanism remains largely unidentified. In this study, we determine the density of trap states in CdTe quantum-dot solids both experimentally, using a combination of electrochemical control of the Fermi level with ultrafast transient absorption and time-resolved photoluminescence spectroscopy, and theoretically, via density functional theory calculations. We find a high density of very efficient electron traps centered ∼0.42 eV above the valence band. Electrochemical filling of these traps increases the electron lifetime and the photoluminescence quantum yield by more than an order of magnitude. The trapping rate constant for holes is an order of magnitude lower that for electrons. These observations can be explained by Auger-mediated electron trapping. From density functional theory calculations we infer that the traps are formed by dicoordinated Te atoms at the quantum dot surface. The combination of our unique experimental determination of the density of trap states with the theoretical modeling of the quantum dot surface allows us to identify the trapping mechanism and chemical reaction at play during charge trapping in these quantum dots.
We show that the activity of cobalt for the oxygen evolution reaction (OER) can be enhanced by confining it in the interlayer region of birnessite (layered manganese oxide). The cobalt intercalation was verified by employing state-of-the-art characterization techniques such as XRD, Raman and electron microscopy. It is demonstrated that the Co 2+ /birnessite electrocatalyst can reach 10 mA cm-2 at an 10
Carbonization of nature-inspired polydopamine can yield thin films with high electrical conductivity. Understanding of the structure of carbonized PDA (cPDA) is therefore highly desired. In this study, neutron diffraction, Raman spectroscopy, and other techniques indicate that cPDA samples are mainly amorphous with some short-range ordering and graphite-like structure that emerges with increasing heat treatment temperature. The electrical conductivity and the Seebeck coefficient show different trends with heat treatment temperature, while the thermal conductivity remains insensitive. The largest room-temperature ZT of 2 × 10 was obtained on samples heat-treated at 800 °C, which is higher than that of reduced graphene oxide.
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