Ultrafast transient absorption measurements have been used to study multiple exciton generation in solutions of PbS nanoparticles vigorously stirred to avoid the effects of photocharging. The threshold and slope efficiency of multiple exciton generation are found to be 2.5 ± 0.2 ×E(g) and 0.34 ± 0.08, respectively. Photoemission measurements as a function of nanoparticle size and ageing show that the position of the valence band maximum is pinned by surface effects, and that a thick layer of surface oxide is rapidly formed at the nanoparticle surfaces on exposure to air.
The composition, crystallinity, morphology, and trap‐state density of halide perovskite thin films critically depend on the nature of the precursor solution. A fundamental understanding of the liquid‐to‐solid transformation mechanism is thus essential to the fabrication of high‐quality thin films of halide perovskite crystals for applications such as high‐performance photovoltaics and is the topic of this Review. The roles of additives on the evolution of coordination complex species in the precursor solutions and the resulting effect on perovskite crystallization are presented. The influence of colloid characteristics, DMF/DMSO‐free solutions and the degradation of precursor solutions on the formation of perovskite crystals are also discussed. Finally, the general formation mechanism of perovskite thin films from precursor solutions is summarized and some questions for further research are provided.
Efficient carrier multiplication in InP nanoparticles is reported; ultrafast transient absorption measurements at the band edge were used to determine the number of excitons per photoexcited nanoparticle for a range of both excitation fluences and photon energies. At photon energies greater than 2.1Ϯ 0.2 times the band gap, an average of more than 1 exciton per photoexcited nanoparticle was found even in the limit of vanishing fluence. The average number of excitons generated by an absorbed photon was measured to be 1.18Ϯ 0.03 for excitation photons with energies 2.6 times the band gap.
An atomistic simulation technique has been used to predict the spatial arrangement of the dopant species sodium, lithium, and chlorine within the zinc oxide lattice. The alkaline oxides are preferentially incorporated via a self-compensating mode, forming interstitial cations which hinder the migration of zinc interstitials and hence slow the degradation of the varistor. The addition of chloride ions is shown to negate this effect by forming sodium and chloride substitutional defects rather than any species involving sodium interstitial ions.
Colloidal quantum dots (CQDs) are promising materials for novel light sources and solar energy conversion. However, trap states associated with the CQD surface can produce non-radiative charge recombination that significantly reduces device performance. Here a facile post-synthetic treatment of CdTe CQDs is demonstrated that uses chloride ions to achieve near-complete suppression of surface trapping, resulting in an increase of photoluminescence (PL) quantum yield (QY) from ca. 5% to up to 97.2 ± 2.5%. The effect of the treatment is characterised by absorption and PL spectroscopy, PL decay, scanning transmission electron microscopy, X-ray diffraction and X-ray photoelectron spectroscopy. This process also dramatically improves the air-stability of the CQDs: before treatment the PL is largely quenched after 1 hour of air-exposure, whilst the treated samples showed a PL QY of nearly 50% after more than 12 hours.
Bright red emission (620-650 nm) from perovskite light-emitting diodes (PeLEDs) is usually achieved via a composition including both bromine and iodine anions, which results in poor performance and stability due to phase separation under operating conditions. Here a large-scale ligand-assisted reprecipitation method is devised with nonpolar solvent that enables the fabrication of CsPbI 3 nanowire clusters, emitting at 600 nm. The blue-shift of this emission relative to that of bulk CsPbI 3 (≈700 nm) is attributed to quantum confinement in nanowires. The growth of the nanowires is along the [011] crystal direction and is vacancy driven, resulting in the healing of surface defects and thereby a high photoluminescence quantum yield of 91%. The clusters with ultralow trap density show remarkable structural and environmental stability. PeLEDs based on these clusters exhibit an external quantum efficiency of 6.2% with Commission Internationale de l'Eclairage coordinates of (0.66, 0.34), and record luminance of 13 644 cd m −2 of red electroluminescence. The half-lifetime under an accelerated stability test is 13.5 min for an unencapsulated device in ambient conditions operating at an initial luminance of 11 500 cd m −2 , which corresponds to an estimated half-lifetime of 694 h at 100 cd m −2 based on acceleration factor obtained by experimental testing.
In a conventional solar cell, the energy of an absorbed photon in excess of the band gap is rapidly lost as heat, and this is one of the main reasons that the theoretical efficiency is limited to ~33%. However, an alternative process, multiple exciton generation (MEG), can occur in colloidal quantum dots. Here, some or all of the excess energy is instead used to promote one or more additional electrons to the conduction band, potentially increasing the photocurrent of a solar cell and thereby its output efficiency. This review will describe the development of this field over the decade since the first experimental demonstration of multiple exciton generation, including the controversies over experimental artefacts, comparison with similar effects in bulk materials, and the underlying mechanisms. We will also describe the current state-of-the-art and outline promising directions for further development.
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