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Publications (56)
Transition metal oxide (TMO) photoabsorbers are expected to play an important role in the development of renewable solar‐to‐fuel devices. Modest efficiencies have been demonstrated with devices based on TMO photoabsorbers, and further progress will likely rely on material property control beyond conventional bulk chemistry or nanostructuring strate...
We measure the mean inner potential (MIP) of hematite, α-Fe2O3, using electron holography and transmission electron microscopy. Since the MIP is sensitive to valence electrons, we propose its use as a chemical bonding parameter for solids. Hematite can test the sensitivity of the MIP as a bonding parameter because of the Morin magnetic phase transi...
Metal oxides are considered as stable and low‐cost photoelectrode candidates for hydrogen production by photoelectrochemical solar water splitting. However, their power conversion efficiencies usually suffer from poor transport of photogenerated charge carriers, which has been attributed previously to a variety of effects occurring on different tim...
External quantum efficiency (EQE) of bismuth vanadate thin film photoanodes, measured in a pH 7 potassium phosphate buffer solution with sodium sulfite hole scavenger, was observed to substantially decrease when measured under white light bias (LB). While the EQE exhibited a fast initial decrease across its full spectral range, a ~3.5 eV (350 nm) f...
Resonant Inelastic X-Ray Scattering (RIXS) spectra of hematite were measured at the Fe L3-edge for heteroepitaxial thin films which were undoped and doped with 1% Ti, Sn or Zn, in the energy loss range in excess of 1 eV to study electronic transitions. The spectra were measured for several momentum transfers (q), conducted at both low temperature (...
The Dzyaloshinskii-Moriya interaction (DMI) is at the heart of many modern developments in the research field of spintronics. DMI is known to generate noncollinear magnetic textures, and can take two forms in antiferromagnets: homogeneous or inter-sublattice, leading to small, canted moments and inhomogeneous or intra-sublattice, leading to formati...
Resonant inelastic x-ray scattering (RIXS) spectra of hematite (α−Fe2O3) were measured at the Fe L3 edge for heteroepitaxial thin films which were undoped and doped with 1% Ti, Sn, or Zn, in the energy-loss range in excess of 1 eV to study electronic transitions. The spectra were measured for several momentum transfers q, conducted at both low temp...
In this paper we review some of the considerations and potential sources of error when conducting Incident Photon to Current Efficiency (IPCE) measurements, with focus on photoelectrochemical (PEC) cells for water splitting. The PEC aspect introduces challenges for accurate measurements often not encountered in dry PV cells. These can include slow...
Photoelectrochemical water splitting as means of producing clean hydrogen fuel has attracted the attention of researchers for nearly 50 years. Since photoelectrochemical cells must operate in a highly corrosive environment, significant efforts have been directed at the development of high efficiency photoelectrodes comprised of transition metal oxi...
Hematite (α-Fe2O3) is a leading photoanode candidate for photoelectrochemical water splitting. Despite extensive research efforts, the champion hematite photoanodes reported to date have achieved less than half of the maximal photocurrent predicted by its bandgap energy. Here we show that this underachievement arises, to a large extent, because of...
The Dzyaloshinskii-Moriya interaction (DMI) is at the heart of many modern developments in the research field of spintronics. DMI is known to generate noncollinear magnetic textures, and can take two forms in antiferromagnets: homogeneous or inter-sublattice, leading to small, canted moments and inhomogeneous or intra-sublattice, leading to formati...
Light absorption in strongly correlated electron materials can excite electrons and holes into a variety of different states. Some of these excitations yield mobile charge carriers, whereas others result in localized states that cannot contribute to photocurrent. The photogeneration yield spectrum, ξ(λ), represents the wavelength-dependent ratio be...
We report room-temperature long-distance spin transport of magnons in antiferromagnetic thin-film hematite doped with Zn. The additional dopants significantly alter the magnetic anisotropies, resulting in a complex equilibrium spin structure that is capable of efficiently transporting spin angular momentum at room temperature without the need for a...
The oxygen evolution reaction (OER) at the surface of semiconductor photoanodes involves photo-generated holes that oxidize water. A certain fraction of the holes that reach the surface recombine with electrons from the conduction band, giving rise to the surface recombination loss. The charge transfer efficiency, xt, defined as the ratio between t...
Strong interference in ultrathin film semiconductor absorbers on metallic back reflectors has been shown to enhance the light harvesting efficiency of solar cell materials. However, metallic back reflectors are not suitable for tandem cell configurations because photons cannot be transmitted through the device. Here, we introduce a method to implem...
Photoelectrochemical impedance spectroscopy (PEIS) is a useful tool for the characterization of photoelectrodes for solar water splitting. However, the analysis of PEIS spectra often involves a priori assumptions that might bias the results. This work puts forward an empirical method that analyzes the distribution of relaxation times (DRT), obtaine...
The spatial collection efficiency portrays the driving forces and loss mechanisms in photovoltaic and photoelectrochemical devices. It is defined as the fraction of photogenerated charge carriers created at a specific point within the device that contribute to the photocurrent. In stratified planar structures, the spatial collection efficiency can...
The photoelectrochemical behavior of a planar 1 cm2 thick Ti-doped hematite film deposited on F:SnO2 coated glass was studied with both front and back illumination. Despite low quantum efficiency, photocurrent was observed upon back illumination with low wavelengths, indicating that some photogenerated holes are able to traverse at least 700 nm acr...
Transparent Fe1-xNixOOH overlayers (~2 nm thick) were deposited photoelectrochemically on (001) oriented heteroepitaxial Sn- and Zn-doped hematite (Fe2O3) thin film photoanodes. In both cases, the water photo-oxidation performance was improved by the co-catalyst overlayers. Intensity modulated photocurrent spectroscopy (IMPS) was applied to study t...
In recent years, hematite potential as a photoanode material for solar hydrogen production has ignited a renewed interest in its physical and interfacial properties, which continues to be an active field of research. Research on hematite photoanodes provides new insights on the correlations between electronic structure, transport properties, excite...
Optimising the photoelectrochemical performance of hematite photoanodes for solar water splitting requires better understanding of the relationships between dopant distribution, structural defects and photoelectrochemical properties. Here, we use complementary characterisation techniques including electron microscopy, conductive atomic force micros...
Optical interference is used to enhance light-matter interaction and harvest broadband light in ultrathin semiconductor absorber films on specular back-reflectors. However, the high-temperature processing in oxygen atmosphere required for oxide absorbers often degrades metallic back-reflectors and their specular reflectance. In order to overcome th...
We report room temperature long-distance spin transport of magnons in antiferromagnetic thin film hematite doped with Zn. The additional dopants significantly alter the magnetic anisotropies, resulting in a complex equilibrium spin structure that is capable of efficiently transporting spin angular momentum at room temperature without the need for a...
Environmental concerns deriving from fossil fuel dependency are driving an energy transition based on sustainable processes to make fuels and chemicals. Solar hydrogen is the pillar of this new green economy, but the technological readiness level of PV electrolysis and direct photoelectrochemical (PEC) electrolysis are still too low to allow broad...
Reading the magnetic state of antiferromagnetic (AFM) thin films is key for AFM spintronic devices. We investigate the underlying physics behind the spin Hall magnetoresistance (SMR) of bilayers of platinum and insulating AFM hematite (α−Fe2O3) and find an SMR efficiency of up to 0.1%, comparable to ferromagnetic-based structures. To understand the...
Reading the magnetic state of antiferromagnetic (AFM) thin films is key for AFM spintronic devices. We investigate the underlying physics behind the spin Hall magnetoresistance (SMR) of bilayers of platinum and insulating AFM hematite ({\alpha}-Fe2O3) and report a record SMR efficiency of up to ~1%. To understand the SMR field dependence, we analys...
Optimising the photoelectrochemical performance of hematite photoanodes for solar water splitting requires better understanding of the relationships between dopant distribution, structural defects and photoelectrochemical properties. Here, we use complementary characterisation techniques including electron microscopy, conductive atomic force micros...
The compensated magnetic order and characteristic, terahertz frequencies of antiferromagnetic materials makes them promising candidates to develop a new class of robust, ultra-fast spintronic devices. The manipulation of antiferromagnetic spin-waves in thin films is anticipated to lead to new exotic phenomena such as spin-superfluidity, requiring a...
For efficient solar water splitting a low cost, stable photoanode is still missing. α-SnWO 4 is a recently found candidate. PEC and IPCE measurements are performed, for different film thicknesses. Thus the optimal film thickness, that is determined is by a tradeoff between a high absorbed light fraction and small charge carrier diffusion length, ca...
Electrolytic hydrogen production faces technological challenges to improve its efficiency, economic value and potential for global integration. In conventional water electrolysis, the water oxidation and reduction reactions are coupled in both time and space, as they occur simultaneously at an anode and a cathode in the same cell. This introduces c...
Spintronics seeks to functionalize antiferromagnetic materials to develop memory and logic devices operating at terahertz speed and robust against external magnetic field perturbations. To be useful, such functionality needs to be developed in thin film devices. The key functionality of long-distance spin-transport has, however, so far only been re...
The charge carrier dynamics of epitaxial hematite films is studied by time‐resolved microwave (TRMC) and time‐resolved terahertz conductivity (TRTC). After excitation with above bandgap illumination, the TRTC signal decays within 3 ps, consistent with previous reports of charge carrier localization times in hematite. The TRMC measurements probe cha...
Strong interference in ultrathin film semiconductor absorbers on metallic back reflectors has been shown to enhance the light harvesting efficiency of solar cell materials. However, metallic back reflectors are not suitable for tandem cell configurations because photons cannot be transmitted through the device. Here, we introduce a method to implem...
H2O2 is a sacrificial reductant that is often used as a hole scavenger to gain insight into photoanode properties. Here we show a distinct mechanism of H2O2 photo-oxidation on haematite (α-Fe2O3) photoanodes. We found that the photocurrent voltammograms display non-monotonous behaviour upon varying the H2O2 concentration, which is not in accord wit...
Optical interference is used to enhance light–matter interaction and harvest broadband light in ultrathin semiconductor absorber films on specular back‐reflectors. However, the high‐temperature processing in oxygen atmosphere required for oxide absorbers often degrades metallic back‐reflectors and their specular reflectance. In order to overcome th...
Photoelectrochemical impedance spectroscopy (PEIS) is a useful tool for the characterization of photoelectrodes for solar water splitting. However, the analysis of PEIS spectra often involves a priori assumptions that might bias the results. This work puts forward an empirical method that analyzes the distribution of relaxation times (DRT), obtaine...
In recent years, hematite's potential as a photoanode material for solar hydrogen production has ignited a renewed interest in its physical and interfacial properties, which continues to be an active field of research. Research on hematite photoanodes provides new insights on the correlations between electronic structure, transport properties, exci...
Transparent Fe1-xNixOOH overlayers (~2 nm thick) were deposited photoelectrochemically on (001) oriented heteroepitaxial Sn- and Zn-doped hematite (α-Fe2O3) thin film photoanodes. In both cases, the water photo-oxidation performance was improved by the co-catalyst overlayers. Intensity modulated photocurrent spectroscopy (IMPS) was applied to study...
The spatial collection efficiency portrays the driving forces and loss mechanisms in photovoltaic and photoelectrochemical devices. It is defined as the fraction of photogenerated charge carriers created at a specific point within the device that contribute to the photocurrent. In stratified planar structures, the spatial collection efficiency can...
The photoelectrochemical behavior of a planar 1 µm thick Ti-doped hematite film deposited on F:SnO2 coated glass was studied with both front and back illumination. Despite low quantum efficiency, photocurrent was observed upon back illumination with low wavelengths, indicating that some photogenerated holes are able to traverse at least 700 nm acro...
The spin states at the surface of epitaxial thin films of hematite, both undoped and doped with 1% Ti, Sn, or Zn, respectively, were probed with x-ray magnetic linear dichroism (XMLD) spectroscopy. Morin transitions were observed for the undoped (TM≈200 K) and Sn-doped (TM≈300 K) cases, while Zn- and Ti-doped samples were always in the high- and lo...
The oxygen evolution reaction (OER) at the surface of semiconductor photoanodes is critical for photoelectrochemical water splitting. This reaction involves photo-generated holes that oxidize water via charge transfer at the...
The orientation dependence on the photoelectrochemical properties of Sn-doped hematite photoanodes was studied by means of heteroepitaxial film growth. Nb-doped SnO2 (NTO) was first grown heteroepitaxially on c, a, r, and m plane single crystal sapphire substrates in three different orientations. Hematite was then grown in the (001), (110), and (10...
Ti-doped, undoped, and Zn-doped hematite (α-Fe2O3) thick (~1 μm) films were found to be n-type, weak n-type, and p-type, respectively. Heterogeneous doping profiles were generated in 30 nm thick hematite stacks on F:SnO2 coated glass substrates with 25 nm thick SnO2 underlayers in order to investigate the effect of different doping profiles on phot...
Heteroepitaxial multilayer Pt(111)/Fe2O3(0001) films were deposited on sapphire c-plane (0001) substrates by RF magnetron sputtering and pulsed laser deposition, respectively. The films were highly crystalline, displaying an in-plane mosaic spread of less than 1° and a homogenous surface morphology with roughness of ∼3 Å. Ellipsometry and UV-vis sp...
One micron thick Gd2O3 films were grown on GaN/AlGaN heterostructures by reactive electron beam physical vapor deposition. The films were of cubic bixbyite phase with strong (222) out-of-plane and in-plane textures. The films showed a columnar microstructure with feather-like growth. Transmission electron microscopy analysis and selected area diffr...
The effects of growth temperature, film thickness, and oxygen flux on the microstructure, phase transition, and interfacial chemistry of gadolinium oxide (Gd{sub 2}O{sub 3}) films grown on Si(111) substrates by electron-beam physical vapor deposition were investigated using a combination of transmission electron microscopy (TEM), electron diffracti...
Thick polycrystalline gadolinium oxide (Gd2O3) films up to 11 μm in thickness were deposited via reactive electron beam-physical vapor deposition (EB-PVD) on silicon (111) substrates for use in neutron radiation detection. The effects of coating thickness, substrate temperature, and oxygen flow on film structural, electrical and optical properties...
A new method for studying the dynamics of a sessile drop by atomic force
microscopy (AFM) is demonstrated. A hydrophobic microsphere (radius, r
=20 micrometers) is brought into contact with a small sessile drop
resting on a hydrophobic surface. When the microsphere touches the
liquid surface, the meniscus rises onto the microsphere due to capillary...
A new method for studying the dynamics of a sessile drop by atomic force microscopy (AFM) is demonstrated. A hydrophobic microsphere (radius, r ∼ 20-30 μm) is brought into contact with a small sessile water drop resting on a polytetrafluoroethylene (PTFE) surface. When the microsphere touches the liquid surface, the meniscus rises onto it because o...