• Energy Research

Heteroepitaxial hematite thin film photoanodes were fabricated, characterized, and shown to be a model system for fundamental studies into solar water splitting.

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 (T_M~200 K) and Sn-doped (T_M~300 K) cases, while Zn and Ti-doped samples were always in the high and low temperature phases, respectively. In contrast to what has been reported for bulk hematite doped with the tetravalent ions Sn4+ and Ti4+, for which T_M dramatically decreases, these dopants substantially increase T_M in thin films, far exceeding the bulk values. The normalized Fe LII-edge dichroism for TT_M state was achieved. The temperature dependence of the critical field for the Sn-doped sample was characterized in detail. It was demonstrated the sample-to-sample variations of the Fe LIII-edge spectra were, for the most part, determined solely by the spin orientation state. Calculations of the polarization-depedent spectra based on a spin-multiplet model were in reasonable agreement with the experiment and showed a mixed excitation character of the peak structures. 8 pages, 8 figures

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 an efficient propagation of spin-waves in thin films. However, the reported decay length in thin films has so far been limited to a few nanometers. In this work, we achieve efficient spin-wave propagation, over micrometer distances, in thin films of the insulating antiferromagnet hematite with large magnetic domains whilst evidencing much shorter attenuation lengths in multidomain thin films. Through transport and magnetic imaging, we conclude on the role of the magnetic domain structure and spin-wave scattering at domain walls to govern the transport. We manipulate the spin transport by tailoring the domain configuration through field cycle training. For the appropriate crystalline orientation, zero-field spin-transport is achieved across micrometers, as required for device integration.

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 challenges, such as product separation, and sets strict constraints on material selection and process conditions. Here, we decouple these reactions by dividing the process into two steps: an electrochemical step that reduces water at the cathode and oxidizes the anode, followed by a spontaneous chemical step that is driven faster at higher temperature, which reduces the anode back to its initial state by oxidizing water. This enables overall water splitting at average cell voltages of 1.44–1.60 V with nominal current densities of 10–200 mA cm−2 in a membrane-free, two-electrode cell. This allows us to produce hydrogen at low voltages in a simple, cyclic process with high efficiency, robustness, safety and scale-up potential. Conventionally, the two half reactions involved in water electrolysis occur simultaneously, presenting materials and process challenges. Here, the authors decouple these to split water efficiently in two steps: electrochemical hydrogen evolution, followed by spontaneous oxygen evolution at elevated temperature.

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 photoelectrochemical performance and compare with homogeneously doped counterpart photoelectrodes. Among the homogeneously doped photoelectrodes, the Ti-doped sample displayed the highest plateau photocurrent but also the highest onset potential, whereas the Zn-doped one had the lowest onset potential and the lowest plateau photocurrent. Heterogeneously doped photoelectrodes displayed both high plateau photocurrent and low onset potential, with the highest performance achieved for the specimen with Ti-doped, undoped, and Zn-doped layers at the bottom, center, and top parts of the stack, respectively. This demonstrates the potential of heterogeneous doping to improve...

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 (��-Fe2O3) and find an SMR efficiency of up to 0.1%, comparable to ferromagnetic based structures. To understand the observed complex SMR field dependence, we analyse the effect of misalignments of the magnetic axis that arise during growth of thin films, by electrical measurements and direct magnetic imaging, and find that a small deviation can result in significant signatures in the SMR response. This highlights the care that must be taken when interpreting SMR measurements on AFM spin textures.