Nicolas Tétreault

Inorganic hole conductor-based lead halide perovskite solar cells with 12.4% conversion efficiency

Organo-lead halide perovskites have attracted much attention for solar cell applications due to their unique optical and electrical properties. With either low-temperature solution processing or vacuum evaporation, the overall conversion efficiencies of perovskite solar cells with organic hole-transporting material were quickly improved to over 15% during the last 2 years. However, the organic hole-transporting materials used are normally quite expensive due to complicated synthetic procedure or high-purity requirement. Here, we demonstrate the application of an effective and cheap inorganic p-type hole-transporting material, copper thiocyanate, on lead halide perovskite-based devices. With low-temperature solution-process deposition method, a power conversion efficiency of 12.4% was achieved under full sun illumination. This work represents a well-defined cell configuration with optimized perovskite morphology by two times of lead iodide deposition, and opens the door for integration of a class of abundant and inexpensive material for photovoltaic application.

Impedance Spectroscopic Analysis of Lead Iodide Perovskite-Sensitized Solid-State Solar Cells

Mesoscopic solid-state solar cells based on the inorganic-organic hybrid perovskite CH3NH3PbI3 in conjunction with the amorphous organic semiconductor spiro-MeOTAD as a hole transport material (HTM) are investigated using impedance spectroscopy (IS). A model to interpret the frequency response of these devices is established by expanding and elaborating on the existing models used for the liquid and solid-state dye-sensitized solar cells. Furthermore, the influence of changing the additive concentrations of tert-butylpyridine and LiTFSI in the HTM and varying the HTM overlayer thickness on top of the sub-micrometer thick TiO2 on the extracted IS parameters is investigated. The internal electrical processes of such devices are studied and correlated with the overall device performance. In particular, the features in the IS responses that are attributed to the ionic and electronic transport properties of the perovskite material and manifest as a slow response at low frequency and an additional RC element at intermediate frequency, respectively, are explored.

Passivating surface states on water splitting hematite photoanodes with alumina overlayers

Hematite is a promising material for inexpensive solar energy conversion viawater splitting but has been limited by the large overpotential (0.5–0.6 V) that must be applied to afford high wateroxidation photocurrent. This has conventionally been addressed by coating it with a catalyst to increase the kinetics of the oxygen evolution reaction. However, surface recombination at trapping states is also thought to be an important factor for the overpotential, and herein we investigate a strategy to passivate trapping states using conformal overlayers applied by atomic layer deposition. While TiO2 overlayers show no beneficial effect, we find that an ultra-thin coating of Al2O3 reduces the overpotential required with state-of-the-art nano-structured photo-anodes by as much as 100 mV and increases the photocurrent by a factor of 3.5 (from 0.24 mA cm−2 to 0.85 mA cm−2) at +1.0 V vs. the reversible hydrogen electrode (RHE) under standard illumination conditions. The subsequent addition of Co2+ ions as a catalyst further decreases the overpotential and leads to a record photocurrent density at 0.9 V vs. RHE (0.42 mA cm−2). A detailed investigation into the effect of the Al2O3 overlayer by electrochemical impedance and photoluminescence spectroscopy reveals a significant change in the surface capacitance and radiative recombination, respectively, which distinguishes the observed overpotential reduction from a catalytic effect and confirms the passivation of surface states. Importantly, this work clearly demonstrates that two distinct loss processes are occurring on the surface of high-performance hematite and suggests a viable route to individually address them.

Cathodic shift in onset potential of solar oxygen evolution on hematite by 13-group oxide overlayers

The onset potential of photoelectrochemical water oxidation on ultrathin hematite was improved by up to 200 mV by the chemical bath deposition of 13-group oxides as overlayers. It is proposed that the corundum-type overlayers released lattice strain of the ultrathin hematite layer and decreased the density of surface states. Particularly, a Ga2O3 overlayer exhibited an enhanced photocurrent attributed to stoichiometric water splitting near the onset potential. The photocurrent was sustained over a day, attesting to its outstanding performance and durability for water splitting.

Novel nanostructures for next generation dye-sensitized solar cells

Herein, we review our latest advancements in nanostructured photoanodes for next generation photovoltaics in general and dye-sensitized solar cells in particular. Bottom-up self-assembly techniques are developed to fabricate large-area 3D nanostructures that enable enhanced charge extraction and light harvesting through optical scattering or photonic crystal effects to improve photocurrent, photovoltage and fill factor. Using generalized techniques to fabricate specialized nanostructures enables specific optoelectronic and physical characteristics like conduction, charge extraction, injection, recombination and light harvesting but also helps improve mechanical flexibility and long-term stability in low cost materials.

High-efficiency dye-sensitized solar cell with three-dimensional photoanode.

Herein, we present a straightforward bottom-up synthesis of a high electron mobility and highly light scattering macroporous photoanode for dye-sensitized solar cells. The dense three-dimensional Al/ZnO, SnO(2), or TiO(2) host integrates a conformal passivation thin film to reduce recombination and a large surface-area mesoporous anatase guest for high dye loading. This novel photoanode is designed to improve the charge extraction resulting in higher fill factor and photovoltage for DSCs. An increase in photovoltage of up to 110 mV over state-of-the-art DSC is demonstrated.

Subnanometer Ga2O3 Tunnelling Layer by Atomic Layer Deposition to Achieve 1.1 V Open-Circuit Potential in Dye-Sensitized Solar Cells

Herein, we present the first use of a gallium oxide tunnelling layer to significantly reduce electron recombination in dye-sensitized solar cells (DSC). The subnanometer coating is achieved using atomic layer deposition (ALD) and leading to a new DSC record open-circuit potential of 1.1 V with state-of-the-art organic D-π-A sensitizer and cobalt redox mediator. After ALD of only a few angstroms of Ga(2)O(3), the electron back reaction is reduced by more than an order of magnitude, while charge collection efficiency and fill factor are increased by 30% and 15%, respectively. The photogenerated exciton separation processes of electron injection into the TiO(2) conduction band and the hole injection into the electrolyte are characterized in detail.

High-efficiency solid-state dye-sensitized solar cells: fast charge extraction through self-assembled 3D fibrous network of crystalline TiO2 nanowires.

Herein, we present a novel morphology for solid-state dye-sensitized solar cells based on the simple and straightforward self-assembly of nanorods into a 3D fibrous network of fused single-crystalline anatase nanowires. This architecture offers a high roughness factor, significant light scattering, and up to several orders of magnitude faster electron transport to reach a near-record-breaking conversion efficiency of 4.9%.

Towards the synthetic all-optical computer: science fiction or reality?

The global race for the optically integrated photonic chip is driven by the prospective that miniaturization of optical devices and enhanced chip functionality may revolutionize the manufacture of optical circuits, and the futuristic dream of the all-optical computer may come true. The aim of this article is to take a brief yet critical look at some developments in microsphere self-assembly of colloidal photonic crystals and their technological potential from the perspective of research results that have recently emerged from our materials chemistry group. The focus of the discussion centers on the provocative vision of the “colloidal photonic crystal micropolis”, Fig. 1, which depicts the direction in which the colloidal photonic crystal research of our materials chemistry group is heading. It is intended to bring to the forefront the pointed question of whether the most recent versions of colloidal photonic crystals and their integration on chips, developed in our laboratory, can rise to the stringent specifications of structural perfection and optical quality, functionality and complexity that will be demanded for photonic crystal optical devices and optical circuits touted for next generation all-optical chip and telecommunication technologies.

A Ga2O3 underlayer as an isomorphic template for ultrathin hematite films toward efficient photoelectrochemical water splitting

Hematite photoanodes for photoelectrochemical (PEC) water splitting are often fabricated as extremely-thin films to minimize charge recombination because of the short diffusion lengths of photoexcited carriers. However, poor crystallinity caused by structural interaction with a substrate negates the potential of ultrathin hematite photoanodes. This study demonstrates that ultrathin Ga2O3 underlayers, which were deposited on conducting substrates prior to hematite layers by atomic layer deposition, served as an isomorphic (corundum-type) structural template for ultrathin hematite and improved the photocurrent onset of PEC water splitting by 0.2 V. The benefit from Ga2O3 underlayers was most pronounced when the thickness of the underlayer was approximately 2 nm. Thinner underlayers did not work effectively as a template presumably because of insufficient crystallinity of the underlayer, while thicker ones diminished the PEC performance of hematite because the underlayer prevented electron injection from hematite to a conductive substrate due to the large conduction band offset. The enhancement of PEC performance by a Ga2O3 underlayer was more significant for thinner hematite layers owing to greater margins for improving the crystallinity of ultrathin hematite. It was confirmed that a Ga2O3 underlayer was applicable to a rough conducting substrate loaded with Sb-doped SnO2 nanoparticles, improving the photocurrent by a factor of 1.4. Accordingly, a Ga2O3 underlayer could push forward the development of host-guest-type nanocomposites consisting of highly-rough substrates and extremely-thin hematite absorbers.