Cation Disorder and Local Structural Distortions in AgxBi1-xS2 Nanoparticles.

By combining X-ray absorption fine structure and X-ray diffraction measurements with density functional and molecular dynamics simulations, we study the structure of a set of AgxBi1-xS2 nanoparticles, a materials system of considerable current interest for photovoltaics. An apparent contradiction between the evidence provided by X-ray absorption and diffraction measurements is solved by means of the simulations. We find that disorder in the cation sublattice induces strong local distortions, leading to the appearance of short Ag-S bonds, the overall lattice symmetry remaining close to hexagonal.

Solution processed infrared- and thermo-photovoltaics based on 0.7 eV bandgap PbS colloidal quantum dots.

Harnessing low energy photons is of paramount importance for multi-junction high efficiency solar cells as well as for thermo-photovoltaic applications. However, semiconductor absorbers with the bandgap lower than 0.8 eV have been limited to III-V (InGaAs) or IV (Ge) semiconductors that are characterized by high manufacturing costs and complicated lattice matching requirements in their growth and integration with higher bandgap cells. Here, we have developed solution processed low bandgap photovoltaic devices based on PbS colloidal quantum dots (CQDs) with a bandgap of 0.7 eV suited for both thermo-photovoltaics and low energy solar photon harvesting. By matching the spectral response of those cells to that of the infrared solar spectrum, we report a record high short circuit current (JSC) of 37 mA cm-2 under the full solar spectrum and 5.5 mA cm-2 when placed at the back of a silicon wafer resulting in power conversion efficiencies (PCEs) of 6.4% and 0.7%, respectively. Moreover, the device reached an above bandgap PCE of ∼6% as a thermo-photovoltaic cell recorded under a 1000 °C blackbody radiator.

Infrared Solution-Processed Quantum Dot Solar Cells Reaching External Quantum Efficiency of 80% at 1.35 µm and Jsc in Excess of 34 mA cm-2.

Developing low-cost photovoltaic absorbers that can harvest the short-wave infrared (SWIR) part of the solar spectrum, which remains unharnessed by current Si-based and perovskite photovoltaic technologies, is a prerequisite for making high-efficiency, low-cost tandem solar cells. Here, infrared PbS colloidal quantum dot (CQD) solar cells employing a hybrid inorganic-organic ligand exchange process that results in an external quantum efficiency of 80% at 1.35 µm are reported, leading to a short-circuit current density of 34 mA cm-2 and a power conversion efficiency (PCE) up to 7.9%, which is a current record for SWIR CQD solar cells. When this cell is placed at the back of an MAPbI3 perovskite film, it delivers an extra 3.3% PCE by harnessing light beyond 750 nm.

Plasmon-Enhanced Energy Transfer in Photosensitive Nanocrystal Device.

Förster resonance energy transfer (FRET) interacted with localized surface plasmon (LSP) gives us the ability to overcome inadequate transfer of energy between donor and acceptor nanocrystals (NCs). In this paper, we show LSP-enhanced FRET in colloidal photosensors of NCs in operation, resulting in substantially enhanced photosensitivity. The proposed photosensitive device is a layered self-assembled colloidal platform consisting of separated monolayers of the donor and the acceptor colloidal NCs with an intermediate metal nanoparticle (MNP) layer made of gold interspaced by polyelectrolyte layers. Using LBL assembly, we fabricated and comparatively studied seven types of such NC-monolayer devices (containing only donor, only acceptor, Au MNP-donor, Au MNP-acceptor, donor-acceptor bilayer, donor-Au MNP-acceptor trilayer, and acceptor-Au MNP-donor reverse trilayer). In these structures, we revealed the effect of LSP-enhanced FRET and exciton interactions from the donor NCs layer to the acceptor NCs layer. Compared to a single acceptor NC device, we observed a significant extension in operating wavelength range and a substantial photosensitivity enhancement (2.91-fold) around the LSP resonance peak of Au MNPs in the LSP-enhanced FRET trilayer structure. Moreover, we present a theoretical model for the intercoupled donor-Au MNP-acceptor structure subject to the plasmon-mediated nonradiative energy transfer. The obtained numerical results are in excellent agreement with the systematic experimental studies done in our work. The potential to modify the energy transfer through mastering the exciton-plasmon interactions and its implication in devices make them attractive for applications in nanophotonic devices and sensors.

Macrocrystals of Colloidal Quantum Dots in Anthracene: Exciton Transfer and Polarized Emission.

In this work, centimeter-scale macrocrystals of nonpolar colloidal quantum dots (QDs) incorporated into anthracene were grown for the first time. The exciton transfer from the anthracene host to acceptor QDs was systematically investigated, and anisotropic emission from the isotropic QDs in the anthracene macrocrystals was discovered. Results showed a decreasing photoluminescence lifetime of the donor anthracene, indicating a strengthening energy transfer with increasing QD concentration in the macrocrystals. With the anisotropy study, QDs inside the anthracene host acquired a polarization ratio of ~1.5 at 0° collection angle, and this increases to ~2.5 at the collection angle of 60°. A proof-of-concept application of these excitonic macrocrystals as tunable color converters on light-emitting diodes was also demonstrated.

Stable and Low-Threshold Optical Gain in CdSe/CdS Quantum Dots: An All-Colloidal Frequency Up-Converted Laser.

An all-solution processed and all-colloidal laser is demonstrated using tailored CdSe/CdS core/shell quantum dots, which exhibit highly stable and low-threshold optical gain owing to substantially suppressed non-radiative Auger recombination.

Mn(2+)-Doped CdSe/CdS Core/Multishell Colloidal Quantum Wells Enabling Tunable Carrier-Dopant Exchange Interactions.

In this work, we report the manifestations of carrier-dopant exchange interactions in colloidal Mn(2+)-doped CdSe/CdS core/multishell quantum wells. The carrier-magnetic ion exchange interaction effects are tunable through wave function engineering. In our quantum well heterostructures, manganese was incorporated by growing a Cd0.985Mn0.015S monolayer shell on undoped CdSe nanoplatelets using the colloidal atomic layer deposition technique. Unlike previously synthesized Mn(2+)-doped colloidal nanostructures, the location of the Mn ions was controlled with atomic layer precision in our heterostructures. This is realized by controlling the spatial overlap between the carrier wave functions with the manganese ions by adjusting the location, composition, and number of the CdSe, Cd1-xMnxS, and CdS layers. The photoluminescence quantum yield of our magnetic heterostructures was found to be as high as 20% at room temperature with a narrow photoluminescence bandwidth of ∼22 nm. Our colloidal quantum wells, which exhibit magneto-optical properties analogous to those of epitaxially grown quantum wells, offer new opportunities for solution-processed spin-based semiconductor devices.

Ultralow Threshold One-Photon- and Two-Photon-Pumped Optical Gain Media of Blue-Emitting Colloidal Quantum Dot Films.

Colloidal quantum dots (QDs) offer advantageous properties as an optical gain media for lasers. Optical gain in the QDs has been shown in the whole visible spectrum, yet it has been intrinsically challenging to realize efficient amplified spontaneous emission (ASE) and lasing in the blue region of the visible spectrum. Here, we synthesize large-sized core/gradient shell CdZnS/ZnS QDs as an efficient optical gain media in the blue spectral range. In this Letter, we demonstrate for the first time that two-photon-absorption-pumped ASE from the blue-emitting QD is achievable with a threshold as low as 6 mJ/cm(2). Utilizing these QDs, we also report one-photon-absorption-pumped ASE at an ultralow threshold of ∼60 µJ/cm(2), which is comparable to the state-of-the-art red-emitting QD-based gain media. This one-photon-pumped ASE threshold is an order of magnitude better than that of the previously reported best blue-emitting QD-based gain media.