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Facile phase selective synthesis of CuInS

Perovskites have quickly become globally renowned for their extremely attractive electronic and optical characteristics. However, a clear relationship between the composition and photoelectronic properties of perovskites is still not well understood, developing this understanding is imperative to designing perovskite devices tailored to suit the needs of the application. In this study we characterize chlorine-doped MAPbI thin films produced by aerosol assisted chemical vapor deposition and compare the composition of the sample series via a comprehensive set of spectroscopy techniques including: Raman, photoluminescence, X-ray photoelectron and ultrafast transient absorption spectroscopy. We discuss the spectral properties revealed and relate our findings to the mechanisms attributed to the impressive optoelectronic properties exhibited by the perovskite structure.

We report on a combined theoretical and experimental study of the impact of alloy fluctuations and Coulomb effects on the electronic and optical properties of \documentclass[12pt]{minimal} \usepackage{amsmath} \usepackage{wasysym} \usepackage{amsfonts} \usepackage{amssymb} \usepackage{amsbsy} \usepackage{mathrsfs} \usepackage{upgreek} \setlength{\oddsidemargin}{-69pt} \begin{document}$$c$$\end{document}c-plane GaN/AlGaN multi-quantum well systems. The presence of carrier localization effects in this system was demonstrated by experimental observations, such as the “S-shape” temperature dependence of the photoluminescence (PL) peak energy, and non-exponential PL decay curves that varied across the PL spectra at 10 K. A three-dimensional modified continuum model, coupled with a self-consistent Hartree scheme, was employed to gain insight into the electronic and optical properties of the experimentally studied \documentclass[12pt]{minimal} \usepackage{amsmath} \usepackage{wasysym} \usepackage{amsfonts} \usepackage{amssymb} \usepackage{amsbsy} \usepackage{mathrsfs} \usepackage{upgreek} \setlength{\oddsidemargin}{-69pt} \begin{document}$$c$$\end{document}c-plane GaN/AlGaN quantum wells. This model confirmed the existence of strong hole localization arising from the combined effects of the built-in polarization field along the growth direction and the alloy fluctuations at the quantum well/barrier interface. However, for electrons these localization effects are less pronounced in comparison to the holes. Furthermore, our calculations show that the attractive Coulomb interaction between electron and hole results in exciton localization. This behavior is in contrast to the picture of independently localized electrons and holes, often used to explain the radiative recombination process in \documentclass[12pt]{minimal} \usepackage{amsmath} \usepackage{wasysym} \usepackage{amsfonts} \usepackage{amssymb} \usepackage{amsbsy} \usepackage{mathrsfs} \usepackage{upgreek} \setlength{\oddsidemargin}{-69pt} \begin{document}$$c$$\end{document}c-plane InGaN/GaN quantum well systems.

Colloidal quantum dots (CQDs) can be used in conjunction with organic charge‐transporting layers to produce light‐emitting diodes, solar cells and other devices. The efficacy of CQDs in these applications is reduced by the non‐radiative recombination associated with surface traps. Here we investigate the effect on the recombination dynamics in CdTe CQDs of the passivation of these surface traps by chloride ions. Radiative recombination dominates in these passivated CQDs, with the radiative lifetime scaling linearly with CQD volume over τr=20–55 ns. Before chloride passivation or after exposure to air, two non‐radiative components are also observed in the recombination transients, with sample‐dependent lifetimes typically of less than 1 ns and a few ns. The non‐radiative dynamics can be explained by Auger‐mediated trapping of holes and the lifetimes of this process calculated by an atomistic model are in agreement with experimental values if assuming surface oxidation of the CQDs.

Colloidal quantum dots (CQDs) are semiconductor crystals, the nanometre-scale size of which both allows their absorption edge to be controlled during growth and enhances the yield of multiple exciton generation. These properties, combined with the facile and scalable solution-phase methods by which they can be made and processed, make CQDs promising candidates for the light-absorbing species in third-generation photovoltaic devices. However, the effectiveness of CQDs in this role depends crucially on the relative rates of a number processes affecting the charges photogenerated in CQDs. We describe the most important of these processes and how they can be optimised to enhance solar cell efficiency by engineering the structure and composition of CQDs.

Achieving control of the surface chemistry of colloidal quantum dots (CQDs) is essential to fully exploit their properties in solar cells, but direct measurement of the chemistry and electronic structure in the outermost atomic layers is challenging. Here we probe the surface oxidation and passivation of cation-exchanged PbS/CdS core/shell CQDs with sub nm-scale precision using synchrotron-radiation-excited depth-profiling photoemission. We investigate the surface composition of the topmost 1-2.5 nm of the CQDs as a function of depth, for CQDs of varying CdS shell thickness, and examine how the surface changes after prolonged air exposure. We demonstrate that the Cd is localized at the surface of the CQDs. The surface-localized products of oxidation are identified, and the extent of oxidation quantified. We show that oxidised sulfur species are progressively eliminated as Cd replaces Pb at the surface. A sub-monolayer surface 'decoration' of Cd is found to be effective in passivating the CQDs. We show that the measured energy-level alignments at PbS/CdS colloidal quantum dot surfaces differ from those expected on the basis of bulk band offsets, and are strongly affected by the oxidation products. We develop a model for the passivating action of Cd. The optimum shell thickness (of around 0.1 nm, previously found to give maximised power conversion efficiency in PbS/CdS solar cells) is found to correspond to a trade-off between the rate of oxidation and the introduction of a surface barrier to charge transport.

We report measurements of multiple exciton generation and recombination in InP/CdS (core/shell) colloidal quantum dots. Ultrafast transient absorption spectroscopy was used to measure the sub-nanosecond charge dynamics for a range of pump fluences and for different pump photon energies. Analysis of the resulting transients was used to determine the quantum yield of multiple exciton generation, which was found to be 1.22 ± 0.01 for a pump photon energy equivalent to three times the band gap.

Ultrafast charge dynamics in dispersions of MoS2 nanosheets in N-methyl-2-pyrrolidone are reported. Samples were prepared by the ultrasonication-assisted exfoliation of MoS2 powder, resulting in nanosheets that were predominantly monolayer and had an average sheet size of 32.4 ± 0.1 nm. These dispersions were characterized using absorption and photoluminescence spectroscopy, transient photoluminescence measurements, and atomic force microscopy before the ultrafast charge dynamics were studied via transient absorption spectroscopy. The transient absorption spectra exhibited bleach peaks and photoinduced absorption peaks in spectral regions corresponding to both the A and B excitons of MoS2. The growth and decay of the features in the B exciton region were determined largely by the dynamics of the exciton population, while the features in the A exciton region depend on the dynamics of both excitons and trions.

The lasing behavior of solution-based colloidal quantum dots within an open microcavity is reported. The small size and wide tunability of the cavity provide single mode lasing over a wavelength range in excess of 25 nm. By extracting the lasing threshold and differential gain for the fundamental cavity mode over this spectral range, gain spectroscopy of the quantum dot solution is demonstrated. This new approach could help in the optimization of laser gain media and provides a way of constructing miniature laser arrays for on-chip integration.

Colloidal quantum dots (CQDs) are promising materials for solar cells because their optoelectronic properties are easily adjusted by control of their size, structure and composition. We present calculations of the band gap and radiative lifetime for varying core diameter and shell thickness of CdSe/CdTe core/shell Type II CQDs using a combination of single particle (2,6)-band k·p and many-electron configuration interaction (CI) Hamiltonians. These calculations are validated by comparison with experimental absorption spectra and photoluminescence decay data. The results are then incorporated into a model of photovoltaic efficiency which demonstrates how the overall performance of a solar cell based on Type II CQDs is affected by changes in the core/shell geometry. The largest effect on photovoltaic efficiency is found to be due to the longer radiative lifetime produced by increasing the shell thickness.

The lasing threshold of the fundamental cavity mode is measured as a function of wavelength and single mode lasing is demonstrated for colloidal CdSe/CdS quantum dots and nanoplaletes using tunable open microcavities.

Sub-nanosecond charge dynamics in monodisperse Au nanoparticles (NPs) supported on TiO2 colloidal spheres are studied as a function of NP diameter using ultrafast transient absorption spectroscopy. The decay of the transmittance changes observed in the region of the plasmon resonance of the Au NPs following photoexcitation of the TiO2 spheres are well-described by a bi-exponential function consisting of a fast component of 2 ps duration associated with electron-phonon scattering, followed by a slow and relatively weak component associated with phonon-phonon scattering. The decay constant characterising the latter component was found to be dependent on the size of the Au NPs, rising from 49 ± 3 to 128 ± 6 ps as the diameter of the Au NPs increased from 12.2 ± 2.2 nm to 24.5 ± 2.8 nm, respectively. This journal is © the Partner Organisations 2014.

Sub-nanosecond charge dynamics in monodisperse Au nanoparticles (NPs) supported on TiO2 colloidal spheres are studied as a function of NP diameter using ultrafast transient absorption spectroscopy. The decay of the transmittance changes observed in the region of the plasmon resonance of the Au NPs following photoexcitation of the TiO2 spheres are well-described by a bi-exponential function consisting of a fast component of 2 ps duration associated with electron-phonon scattering, followed by a slow and relatively weak component associated with phonon-phonon scattering. The decay constant characterising the latter component was found to be dependent on the size of the Au NPs, rising from 49 ± 3 to 128 ± 6 ps as the diameter of the Au NPs increased from 12.2 ± 2.2 nm to 24.5 ± 2.8 nm, respectively.

We report the optical measurement of the spin dynamics at elevated temperatures and in zero magnetic field for two types of degenerately doped n-InSb quantum wells (QWs), one asymmetric (sample A) and one symmetric (sample B) with regards to the electrostatic potential across the QW. Making use of three directly determined experimental parameters: the spin lifetime, τ(s), the sheet carrier concentration, n, and the electron mobility, μ, we directly extract the zero-field spin splitting. For the asymmetric sample where the Rashba interaction is the dominant source of spin splitting, we deduce a room temperature Rashba parameter of α = 0.09 ± 0.1 eV Å which is in good agreement with calculations and we estimate the Rashba coefficient α(0) (a figure of merit for the ease with which electron spins can be modulated via an electric field). We review the merits/limitations of this approach and the implications of our findings for spintronic devices.

Electron spin relaxation times have been measured in InSb and InAs epilayers in a moderate (

Biomimetic sulfur-deficient indium sulfide (In2.77S4) was synthesized by a template-assisted hydrothermal method using leaves of Mimosa pudica as a template for the first time. The effect of this template in modifying the morphology of the semiconductor particles was determined by physicochemical characterization, revealing an increase in surface area, decrease in microsphere size and pore size and an increase in pore volume density in samples synthesized with the template. X-ray photoelectron spectroscopy (XPS) analysis showed the presence of organic sulfur (S O/S C/S H) and sulfur oxide species ( SO2, SO32−, SO42−) at the surface of the indium sulfide in samples synthesized with the template. Biomimetic indium sulfide also showed significant amounts of Fe introduced as a contaminant present on the Mimosa pudica leaves. The presence of these sulfur and iron species favors the photocatalytic activity for hydrogen production by their acting as a sacrificial reagent and promoting water oxidation on the surface of the templated particles, respectively. The photocatalytic hydrogen production rates over optimally-prepared biomimetic indium sulfide and indium sulfide synthesized without the organic template were 73 and 22 μmol g−1, respectively, indicating an improvement by a factor of three in the templated sample.

Ultrafast transient absorption spectroscopy is used to investigate sub-nanosecond exciton dynamics in CdxHg(1-x)Te alloy colloidal quantum dots. A bleach was observed at the band gap due to state-filling, the mono-exponential decay of which had a characteristic lifetime of 91±1 ps and was attributed to biexciton recombination; no evidence of surface-related trapping was observed. The rise time of the bleach, which is determined by the rate at which hot electrons cool to the band-edge, ranged between 1 and 5 ps depending on the pump photon energy. Measuring the magnitude of the bleach decay for different pump fluences and wavelengths allowed the quantum yield of multiple exciton generation to be determined, and was 115±1% for pump photons with energy equivalent to 2.6 times the band gap.