Jack A. Alexander-Webber

Low-temperature processed electron collection layers of graphene/TiO2 nanocomposites in thin film perovskite solar cells.

The highest efficiencies in solution-processable perovskite-based solar cells have been achieved using an electron collection layer that requires sintering at 500 °C. This is unfavorable for low-cost production, applications on plastic substrates, and multijunction device architectures. Here we report a low-cost, solution-based deposition procedure utilizing nanocomposites of graphene and TiO2 nanoparticles as the electron collection layers in meso-superstructured perovskite solar cells. The graphene nanoflakes provide superior charge-collection in the nanocomposites, enabling the entire device to be fabricated at temperatures no higher than 150 °C. These solar cells show remarkable photovoltaic performance with a power conversion efficiency up to 15.6%. This work demonstrates that graphene/metal oxide nanocomposites have the potential to contribute significantly toward the development of low-cost solar cells.

Mesoporous TiO2 single crystals delivering enhanced mobility and optoelectronic device performance

Mesoporous ceramics and semiconductors enable low-cost solar power, solar fuel, (photo)catalyst and electrical energy storage technologies. State-of-the-art, printable high-surface-area electrodes are fabricated from thermally sintered pre-formed nanocrystals. Mesoporosity provides the desired highly accessible surfaces but many applications also demand long-range electronic connectivity and structural coherence. A mesoporous single-crystal (MSC) semiconductor can meet both criteria. Here we demonstrate a general synthetic method of growing semiconductor MSCs of anatase TiO2 based on seeded nucleation and growth inside a mesoporous template immersed in a dilute reaction solution. We show that both isolated MSCs and ensembles incorporated into films have substantially higher conductivities and electron mobilities than does nanocrystalline TiO2. Conventional nanocrystals, unlike MSCs, require in-film thermal sintering to reinforce electronic contact between particles, thus increasing fabrication cost, limiting the use of flexible substrates and precluding, for instance, multijunction solar cell processing. Using MSC films processed entirely below 150 °C, we have fabricated all-solid-state, low-temperature sensitized solar cells that have 7.3 per cent efficiency, the highest efficiency yet reported. These high-surface-area anatase single crystals will find application in many different technologies, and this generic synthetic strategy extends the possibility of mesoporous single-crystal growth to a range of functional ceramics and semiconductors.

Ultrasmooth organic–inorganic perovskite thin-film formation and crystallization for efficient planar heterojunction solar cells

To date, there have been a plethora of reports on different means to fabricate organic-inorganic metal halide perovskite thin films; however, the inorganic starting materials have been limited to halide-based anions. Here we study the role of the anions in the perovskite solution and their influence upon perovskite crystal growth, film formation and device performance. We find that by using a non-halide lead source (lead acetate) instead of lead chloride or iodide, the perovskite crystal growth is much faster, which allows us to obtain ultrasmooth and almost pinhole-free perovskite films by a simple one-step solution coating with only a few minutes annealing. This synthesis leads to improved device performance in planar heterojunction architectures and answers a critical question as to the role of the anion and excess organic component during crystallization. Our work paves the way to tune the crystal growth kinetics by simple chemistry.

Structured Organic-Inorganic Perovskite toward a Distributed Feedback Laser.

A general strategy for the in-plane structuring of organic-inorganic perovskite films is presented. The method is used to fabricate an industrially relevant distributed feedback (DFB) cavity, which is a critical step toward all-electrially pumped injection laser diodes. This approach opens the prospects of perovskite materials for much improved optical control in LEDs, solar cells, and also toward applications as optical devices.

Weak localization scattering lengths in epitaxial, and CVD graphene

Weak localization in graphene is studied as a function of carrier density in the range from 1 x 10(11) cm(-2) to 1.43 x 10(13) cm(-2) using devices produced by epitaxial growth onto SiC and CVD growth on thin metal film. The magnetic field dependent weak localization is found to be well fitted by theory, which is then used to analyze the dependence of the scattering lengths L-phi, L-i, and L-* on carrier density. We find no significant carrier dependence for L-phi, a weak decrease for L-i with increasing carrier density just beyond a large standard error, and a n(-1/4) dependence for L-*. We demonstrate that currents as low as 0.01 nA are required in smaller devices to avoid hot-electron artifacts in measurements of the quantum corrections to conductivity.

Rapid epitaxy-free graphene synthesis on silicidated polycrystalline platinum

Large-area synthesis of high-quality graphene by chemical vapour deposition on metallic substrates requires polishing or substrate grain enlargement followed by a lengthy growth period. Here we demonstrate a novel substrate processing method for facile synthesis of mm-sized, single-crystal graphene by coating polycrystalline platinum foils with a silicon-containing film. The film reacts with platinum on heating, resulting in the formation of a liquid platinum silicide layer that screens the platinum lattice and fills topographic defects. This reduces the dependence on the surface properties of the catalytic substrate, improving the crystallinity, uniformity and size of graphene domains. At elevated temperatures growth rates of more than an order of magnitude higher (120 μm min−1) than typically reported are achieved, allowing savings in costs for consumable materials, energy and time. This generic technique paves the way for using a whole new range of eutectic substrates for the large-area synthesis of 2D materials.

Hot carrier relaxation of Dirac fermions in bilayer epitaxial graphene

Energy relaxation of hot Dirac fermions in bilayer epitaxial graphene is experimentally investigated by magnetotransport measurements on Shubnikov-de Haas oscillations and weak localization. The hot-electron energy loss rate is found to follow the predicted Bloch-Grüneisen power-law behaviour of T(4) at carrier temperatures from 1.4 K up to ∼100 K, due to electron-acoustic phonon interactions with a deformation potential coupling constant of 22 eV. A carrier density dependence n(e)(-1.5) in the scaling of the T(4) power law is observed in bilayer graphene, in contrast to the n(e)(-0.5) dependence in monolayer graphene, leading to a crossover in the energy loss rate as a function of carrier density between these two systems. The electron-phonon relaxation time in bilayer graphene is also shown to be strongly carrier density dependent, while it remains constant for a wide range of carrier densities in monolayer graphene. Our results and comparisons between the bilayer and monolayer exhibit a more comprehensive picture of hot carrier dynamics in graphene systems.

Parameter Space of Atomic Layer Deposition of Ultrathin Oxides on Graphene

Atomic layer deposition (ALD) of ultrathin aluminum oxide (AlOx) films was systematically studied on supported chemical vapor deposition (CVD) graphene. We show that by extending the precursor residence time, using either a multiple-pulse sequence or a soaking period, ultrathin continuous AlOx films can be achieved directly on graphene using standard H2O and trimethylaluminum (TMA) precursors even at a high deposition temperature of 200 °C, without the use of surfactants or other additional graphene surface modifications. To obtain conformal nucleation, a precursor residence time of >2s is needed, which is not prohibitively long but sufficient to account for the slow adsorption kinetics of the graphene surface. In contrast, a shorter residence time results in heterogeneous nucleation that is preferential to defect/selective sites on the graphene. These findings demonstrate that careful control of the ALD parameter space is imperative in governing the nucleation behavior of AlOx on CVD graphene. We consider our results to have model system character for rational two-dimensional (2D)/non-2D material process integration, relevant also to the interfacing and device integration of the many other emerging 2D materials.

Encapsulation of graphene transistors and vertical device integration by interface engineering with atomic layer deposited oxide

We demonstrate a simple, scalable approach to achieve encapsulated graphene transistors with negligible gate hysteresis, low doping levels and enhanced mobility compared to as-fabricated devices. We engineer the interface between graphene and atomic layer deposited (ALD) Al

Hyperspectral imaging of exciton photoluminescence in individual carbon nanotubes controlled by high magnetic fields.

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