Olivier Ouellette

Fast and Sensitive Solution-Processed Visible-Blind Perovskite UV Photodetectors

The first visible-blind UV photodetector based on MAPbCl3 integrated on a substrate exhibits excellent performance, with responsivities reaching 18 A W(-1) below 400 nm and imaging-compatible response times of 1 ms. This is achieved by using substrate-integrated single crystals, thus overcoming the severe limitations affecting thin films and offering a new application of efficient, solution-processed, visible-transparent perovskite optoelectronics.

Engineering of CH3NH3PbI3 Perovskite Crystals by Alloying Large Organic Cations for Enhanced Thermal Stability and Transport Properties

The number of studies on organic-inorganic hybrid perovskites has soared in recent years. However, the majority of hybrid perovskites under investigation are based on a limited number of organic cations of suitable sizes, such as methylammonium and formamidinium. These small cations easily fit into the perovskites three-dimensional (3D) lead halide framework to produce semiconductors with excellent charge transport properties. Until now, larger cations, such as ethylammonium, have been found to form 2D crystals with lead halide. Here we show for the first time that ethylammonium can in fact be incorporated coordinately with methylammonium in the lattice of a 3D perovskite thanks to a balance of opposite lattice distortion strains. This inclusion results in higher crystal symmetry, improved material stability, and markedly enhanced charge carrier lifetime. This crystal engineering strategy of balancing opposite lattice distortion effects vastly increases the number of potential choices of organic cations for 3D perovskites, opening up new degrees of freedom to tailor their optoelectronic and environmental properties.

Ultralow Self-Doping in Two-dimensional Hybrid Perovskite Single Crystals

Unintentional self-doping in semiconductors through shallow defects is detrimental to optoelectronic device performance. It adversely affects junction properties and it introduces electronic noise. This is especially acute for solution-processed semiconductors, including hybrid perovskites, which are usually high in defects due to rapid crystallization. Here, we uncover extremely low self-doping concentrations in single crystals of the two-dimensional perovskites (C6H5C2H4NH3)2PbI4·(CH3NH3PbI3)n-1 (n = 1, 2, and 3), over three orders of magnitude lower than those of typical three-dimensional hybrid perovskites, by analyzing their conductivity behavior. We propose that crystallization of hybrid perovskites containing large organic cations suppresses defect formation and thus favors a low self-doping level. To exemplify the benefits of this effect, we demonstrate extraordinarily high light-detectivity (1013 Jones) in (C6H5C2H4NH3)2PbI4·(CH3NH3PbI3)n-1 photoconductors due to the reduced electronic noise, which makes them particularly attractive for the detection of weak light signals. Furthermore, the low self-doping concentration reduces the equilibrium charge carrier concentration in (C6H5C2H4NH3)2PbI4·(CH3NH3PbI3)n-1, advantageous in the design of p-i-n heterojunction solar cells by optimizing band alignment and promoting carrier depletion in the intrinsic perovskite layer, thereby enhancing charge extraction.

Single-step colloidal quantum dot films for infrared solar harvesting

Semiconductors with bandgaps in the near- to mid-infrared can harvest solar light that is otherwise wasted by conventional single-junction solar cell architectures. In particular, colloidal quantum dots (CQDs) are promising materials since they are cost-effective, processed from solution, and have a bandgap that can be tuned into the infrared (IR) via the quantum size effect. These characteristics enable them to harvest the infrared portion of the solar spectrum to which silicon is transparent. To date, IR CQD solar cells have been made using a wasteful and complex sequential layer-by-layer process. Here, we demonstrate ∼1 eV bandgap solar-harvesting CQD films deposited in a single step. By engineering a fast-drying solvent mixture for metal iodide-capped CQDs, we deposited active layers greater than 200 nm in thickness having a mean roughness less than 1 nm. We integrated these films into infrared solar cells that are stable in air and exhibit power conversion efficiencies of 3.5% under illumination by t...

Nanoimprint-Transfer-Patterned Solids Enhance Light Absorption in Colloidal Quantum Dot Solar Cells

Colloidal quantum dot (CQD) materials are of interest in thin-film solar cells due to their size-tunable bandgap and low-cost solution-processing. However, CQD solar cells suffer from inefficient charge extraction over the film thicknesses required for complete absorption of solar light. Here we show a new strategy to enhance light absorption in CQD solar cells by nanostructuring the CQD film itself at the back interface. We use two-dimensional finite-difference time-domain (FDTD) simulations to study quantitatively the light absorption enhancement in nanostructured back interfaces in CQD solar cells. We implement this experimentally by demonstrating a nanoimprint-transfer-patterning (NTP) process for the fabrication of nanostructured CQD solids with highly ordered patterns. We show that this approach enables a boost in the power conversion efficiency in CQD solar cells primarily due to an increase in short-circuit current density as a result of enhanced absorption through light-trapping.

2D matrix engineering for homogeneous quantum dot coupling in photovoltaic solids

Colloidal quantum dots (CQDs) are promising photovoltaic (PV) materials because of their widely tunable absorption spectrum controlled by nanocrystal size1,2. Their bandgap tunability allows not only the optimization of single-junction cells, but also the fabrication of multijunction cells that complement perovskites and silicon3. Advances in surface passivation2,4–7, combined with advances in device structures8, have contributed to certified power conversion efficiencies (PCEs) that rose to 11% in 20169. Further gains in performance are available if the thickness of the devices can be increased to maximize the light harvesting at a high fill factor (FF). However, at present the active layer thickness is limited to ~300 nm by the concomitant photocarrier diffusion length. To date, CQD devices thicker than this typically exhibit decreases in short-circuit current (JSC) and open-circuit voltage (VOC), as seen in previous reports3,9–11. Here, we report a matrix engineering strategy for CQD solids that significantly enhances the photocarrier diffusion length. We find that a hybrid inorganic–amine coordinating complex enables us to generate a high-quality two-dimensionally (2D) confined inorganic matrix that programmes internanoparticle spacing at the atomic scale. This strategy enables the reduction of structural and energetic disorder in the solid and concurrent improvements in the CQD packing density and uniformity. Consequently, planar devices with a nearly doubled active layer thicknesses (~600 nm) and record values of JSC (32 mA cm−2) are fabricated. The VOC improved as the current was increased. We demonstrate CQD solar cells with a certified record efficiency of 12%.A new matrix engineering strategy enables improvements of CQD solar cell efficiency via considerable enhancement of the photocarrier diffusion length.

Enhanced Open-Circuit Voltage in Colloidal Quantum Dot Photovoltaics via Reactivity-Controlled Solution-Phase Ligand Exchange

The energy disorder that arises from colloidal quantum dot (CQD) polydispersity limits the open-circuit voltage (VOC ) and efficiency of CQD photovoltaics. This energy broadening is significantly deteriorated today during CQD ligand exchange and film assembly. Here, a new solution-phase ligand exchange that, via judicious incorporation of reactivity-engineered additives, provides improved monodispersity in final CQD films is reported. It has been found that increasing the concentration of the less reactive species prevents CQD fusion and etching. As a result, CQD solar cells with a VOC of 0.7 V (vs 0.61 V for the control) for CQD films with exciton peak at 1.28 eV and a power conversion efficiency of 10.9% (vs 10.1% for the control) is achieved.

Halide Re-Shelled Quantum Dot Inks for Infrared Photovoltaics

Colloidal quantum dots are promising materials for tandem solar cells that complement silicon and perovskites. These devices are fabricated from solution phase; however, existing methods for making infrared-bandgap CQD inks suffer agglomeration and fusion during solution exchange. Here we develop a ligand exchange that provides robust surface protection and thereby avoids aggregation. First, we exchanged long oleic acid ligands to a mixed system comprising medium-chain ammonium and anionic chloride ligands; we then reshelled the surface using short halides and pseudohalide ligands that enabled transfer to a polar solvent. Absorbance and photoluminescence measurements reveal the retention of exciton sharpness, whereas X-ray photoelectron spectroscopy indicates halide capping. The best power conversion efficiency of these devices is 0.76 power points after filtering through silicon, which is 1.9× higher than previous single-step solution-processed IR-CQD solar cells.

Analysis and Experimental Study of Magnetic-Field Amplification by a Double Coil

We investigated the amplification of the magnetic field generated by a floating coil placed in resonance with a driving coil connected to a signal source. With this method, the magnetic field can be amplified without increasing power consumption of the signal source. From an equivalent-circuit model composed of the floating and driving coils, we derived useful formulae for maximizing the magnetic-field amplitude at an arbitrary target frequency. The validity of the formulae was experimentally demonstrated. It was found that under specific conditions, the current induced in the floating coil can be increased by more than one order of magnitude compared to the current in the driving coil, leading to amplification of the magnetic field that reaches 22 dB at the target frequency of 10 MHz without increasing power consumption. We also found that the floating coil is effective in suppressing undesirable magnetic field components originating from common-mode currents. These results pave the way to further reduction of the power consumption in wireless communication schemes such as near field communication.

Multibandgap quantum dot ensembles for solar-matched infrared energy harvesting

As crystalline silicon solar cells approach in efficiency their theoretical limit, strategies are being developed to achieve efficient infrared energy harvesting to augment silicon using solar photons from beyond its 1100 nm absorption edge. Herein we report a strategy that uses multi-bandgap lead sulfide colloidal quantum dot (CQD) ensembles to maximize short-circuit current and open-circuit voltage simultaneously. We engineer the density of states to achieve simultaneously a large quasi-Fermi level splitting and a tailored optical response that matches the infrared solar spectrum. We shape the density of states by selectively introducing larger-bandgap CQDs within a smaller-bandgap CQD population, achieving a 40 meV increase in open-circuit voltage. The near-unity internal quantum efficiency in the optimized multi-bandgap CQD ensemble yielded a maximized photocurrent of 3.7 ± 0.2 mA cm−2. This provides a record for silicon-filtered power conversion efficiency equal to one power point, a 25% (relative) improvement compared to the best previously-reported results.Efficient harvest of solar energy beyond the silicon absorption edge of 1100 nm by semiconductor solar cells remains a challenge. Here Sun et al. mix high multi-bandgap lead sulfide colloidal quantum dot ensembles to further increase both short circuit current and open circuit voltage.