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Register a new userEnhanced Solar Water Splitting by Swift Charge Separation in Au/FeOOH Sandwiched Single Crystalline Fe$_2$O$_3$ Nanoflake Photoelectrodes
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In this work, single crystalline $alpha$-Fe$_2$O$_3$ nanoflakes (NFs) are formed in a highly dense array by Au seeding of a Fe substrate by a thermal oxidation technique. The NFs are conformally decorated with a thin FeOOH cocatalyst layer. Photoelectrochemical (PEC) measurements show that this photoanode with the $alpha$-Fe$_2$O$_3$/FeOOH NFs rooted on the Au/Fe structure exhibits a significantly enhanced PEC water oxidation performance compared to the plain $alpha$-Fe$_2$O$_3$ nanostructure on the Fe substrate. The $alpha$-Fe$_2$O$_3$/FeOOH NFs on Au/Fe photoanode yields a photocurrent density of 3.1 mA cm-2 at 1.5 VRHE, and a remarkably low onset potential of 0.5-0.6 VRHE in 1 M KOH under AM 1.5G (100 mW cm-2) simulated sunlight illumination. The enhancement in PEC performance can be attributed to a synergistic effect of the FeOOH top decoration and Au under-layer. While FeOOH facilitates hole transfer at the interface of electrode/electrolyte, the Au layer provides a sink for the electron transport to the back contact: this leads overall to a drastically improved charge-separation efficiency in the single crystalline $alpha$-Fe$_2$O$_3$ NF photoanode.
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Gallium oxide films were grown by HVPE on (0001) sapphire substrates with and without $alpha$-Cr$_2$O$_3$ buffer produced by RF magnetron sputtering. Deposition on bare sapphire substrates resulted in a mixture of $alpha$-Ga$_2$O$_3$ and $epsilon$-Ga$_2$O$_3$ phases with a dislocation density of about $2cdot10^{10}$ cm$^{-2}$. The insertion of $alpha$-Ga$_2$O$_3$ buffer layers resulted in phase-pure $alpha$-Ga$_2$O$_3$ films and a fourfold reduction of the dislocation density to $5 cdot 10^9$ cm$^{-2}$.
Au nanoparticles at the TiO$_2$ surface can enhance the photocatalytic H$_2$ generation performances owing to their electron transfer co-catalytic ability. Key to maximize the co-catalytic effect is a fine control over Au nanoparticle size and placement on the photocatalyst, in relation to parameters such as the TiO$_2$ morphology, illumination wavelength and pathway, and light penetration depth in the photocatalyst. Here we present an approach for site-selective intrinsic-decoration of anodic TiO$_2$ nanotubes (TNs) with Au nanoparticles: we produce, by Ti and Au co-sputtering, Ti-Au alloy layers that feature compositional gradients across their thickness; these layers, when anodized under self-ordering electrochemical conditions, can form Au-decorated TNs where the Au nanoparticle density and placement vary according to the Au concentration profile in the metal alloy substrates. Our results suggest that, the Au co-catalyst placement strongly affects the photocatalytic H$_2$ evolution performance of the TNs layers. We demonstrate that, when growing Au-decorated TNs, the use of Ti-Au substrates with a suitable Au compositional gradient can lead to higher H$_2$ evolution rates compared to TNs classically grown with a homogenous co-catalyst decoration. As a side effect, a proper placement of the co-catalyst nanoparticles allows for reducing the amount of noble metal without dumping the H$_2$ evolution activity.
Surface electronic structures of the photoelectrodes determine the activity and efficiency of the photoelectrochemical water splitting, but the controls of their surface structures and interfacial chemical reactions remain challenging. Here, we use ferroelectric BiFeO3 as a model system to demonstrate an efficient and controllable water splitting reaction by large-area constructing the hydroxyls-bonded surface. The up-shift of band edge positions at this surface enables and enhances the interfacial holes and electrons transfer through the hydroxyl-active-sites, leading to simultaneously enhanced oxygen and hydrogen evolutions. Furthermore, printing of ferroelectric super-domains with microscale checkboard up/down electric fields separates the distribution of reduction/oxidation catalytic sites, enhancing the charge separation and giving rise to an order of magnitude increase of the photocurrent. This large-area printable ferroelectric surface and super-domains offer an alternative platform for controllable and high-efficient photocatalysis.
We report on the study of optical properties of mist CVD grown alpha Gallium oxide with the observation of excitonic absorption in spectral responsivity measurements. 163 nm of Gallium oxide was grown on sapphire using Gallium acetylacetonate as the starting solution at a substrate temperature of 450 deg C. The film was found to be crystalline and of alpha phase with an on axis full width at half maximum of 92 arcsec as confirmed from X ray diffraction scans. The Taucs plot extracted from absorption spectroscopy exhibited two transitions in the UV regime at 5.3 eV and 5.6 eV, corresponding to excitonic absorption and direct band to band transition respectively. The binding energy of exciton was extracted to be 114 meV from spectral responsivity measurements. Further, metal semiconductor metal photodetectors with lateral inter digitated geometry were fabricated on the film. A sharp band edge was observed at 230 nm in the spectral response with peak responsivity of around 1 Amperes per Watt at a bias of 20 V. The UV to visible rejection ratio was found to be around 100 while the dark current was measured to be around 0.1 nA.
$beta$-Ga$_2$O$_3$ is a next-generation ultra wide bandgap semiconductor (E$_g$ = 4.8 eV to 4.9 eV) that can be homoepitaxially grown on commercial substrates, enabling next-generation power electronic devices among other important applications. Analyzing the quality of deposited homoepitaxial layers used in such devices is challenging, in part due to the large probing depth in traditional x-ray diffraction (XRD) and also due to the surface-sensitive nature of atomic force microscopy (AFM). Here, a combination of evanescent grazing-incidence skew asymmetric XRD and AFM are investigated as an approach to effectively characterize the quality of homoepitaxial $beta$-Ga$_2$O$_3$ layers grown by molecular beam epitaxy at a variety of Ga/O flux ratios. Accounting for both structure and morphology, optimal films are achieved at a Ga/O ratio of $sim$1.15, a conclusion that would not be possible to achieve by either XRD or AFM methods alone. Finally, fabricated Schottky barrier diodes with thicker homoepitaxial layers are characterized by $J-V$ and $C-V$ measurements, revealing an unintentional doping density of 4.3 $times$ 10$^{16}$ cm$^{-3}$ - 2 $times$ 10$^{17}$ cm$^{-3}$ in the epilayer. These results demonstrate the importance of complementary measurement methods for improving the quality of the $beta$-Ga$_2$O$_3$ homoepitaxial layers used in power electronic and other devices.
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