In searching for alternative oxygen evolution reaction (OER) catalysts for acidic water splitting, fast screening of the material intrinsic activity and stability in half-cell tests is of vital importance. The screening process significantly accelerates the discovery of new promising materials without the need of time-consuming real-cell analysis. In commonly employed tests, a conclusion on the catalyst stability is drawn solely on the basis of electrochemical data, for example, by evaluating potential-versus-time profiles. Herein important limitations of such approaches, which are related to the degradation of the backing electrode material, are demonstrated. State-of-the-art Ir-black powder is investigated for OER activity and for dissolution as a function of the backing electrode material. Even at very short time intervals materials like glassy carbon passivate, increasing the contact resistance and concealing the degradation phenomena of the electrocatalyst itself. Alternative backing electrodes like gold and boron-doped diamond show better stability and are thus recommended for short accelerated aging investigations. Moreover, parallel quantification of dissolution products in the electrolyte is shown to be of great importance for comparing OER catalyst feasibility.

Atomic defects in wide band gap materials show great promise for development of a new generation of quantum information technologies, but have been hampered by the inability to produce and engineer the defects in a controlled way. The nitrogen-vacancy (NV) color center in diamond is one of the foremost candidates, with single defects allowing optical addressing of electron spin and nuclear spin degrees of freedom with potential for applications in advanced sensing and computing. Here we demonstrate a method for the deterministic writing of individual NV centers at selected locations with high positioning accuracy using laser processing with online fluorescence feedback. This method provides a new tool for the fabrication of engineered materials and devices for quantum technologies and offers insight into the diffusion dynamics of point defects in solids. Main Text:The engineering of materials at the scale of individual atoms has long been viewed as a holy grail of technology. With the extreme miniaturization of modern semiconductor technology to sub-10 nm feature sizes and the emerging promise of quantum technologies that rely inherently on the principles of quantum physics, the ability to fabricate and manipulate atomic-scale systems is becoming increasingly important.One promising approach to quantum technologies is the use of 'color center' point defects in wide band gap materials that display strong optical transitions, allowing the addressing of single atoms using optical wavelengths within the transparency window of the solid. Fluorescence from single color centers displays quantum statistics with potential for use in communications, sensingWe would like to acknowledge DeBeers and Element Six for providing suitably characterized diamond samples for this work, and in particular Daniel Twitchen and David Fisher for their comments on the manuscript. Data reported in the paper are presented in the Supplementary Materials and are archived at (tbc). The work was funded by the UK Engineering and Physical Sciences Research Council (EPSRC) through the UK hub in Networked Quantum Information Technologies (NQIT), grant # EP/M013243/1. Y-CC, B Griffiths and SN carried out the experiments and performed the data analysis with supervision from JS and PS; B Griffiths, LW, SJ and PS constructed the laser writing and fluorescence feedback apparatus; SI, YL, CJS and BLG carried out the Hahn echo and spatial localization measurements under the supervision of GM and MN; and JS, YCC, PS and MB conceived the experiment; all authors contributed to writing the manuscript. Supplementary Materials: Materials and Methods:The samples used were single-crystal type 1b diamond with nitrogen concentration of 1.8 ppm, produced by a High Pressure High Temperature (HPHT) technique. The diamond was cut and polished with flat surfaces parallel to the (110) plane of the cubic crystal.The optical layout for the combined laser processing and fluorescence feedback apparatus is shown in Figure S1. The laser processing was performed using a regenerat...

Hexagonal boron nitride nanowall thin films were deposited on Si(100) substrates using a Ar(51%)/N2(44%)/H2(5%) gas mixture by unbalanced radio frequency sputtering. The effects of various target-to-substrate distances, substrate temperatures, and substrate tilting angles were investigated. When the substrate is close to the target, hydrogen etching plays a significant role in the film growth, while the effect is negligible for films deposited at a farther distance. The relative quantity of defects was measured by a non-destructive infrared spectroscopy technique that characterized the hydrogen incorporation at dangling nitrogen bonds at defect sites in the deposited films. Despite the films deposited at different substrate tilting angles, the nanowalls of those films were found to consistently grow vertical to the substrate surface, independent of the tilting angle. This implies that chemical processes, rather than physical ones, govern the growth of the nanowalls. The results also reveal that the degree of nanowall crystallization is tunable by varying the growth parameters. Finally, evidence of hydrogen desorption during vacuum annealing is given based on measurements of infrared stretching (E 1u) and bending (A 2u) modes of the optical phonons, and the H–N vibration mode.

Well-defined covalent surface functionalization of diamond is a crucial, yet non-trivial, matter because of diamonds intrinsic chemical inertness and stability. Herein, we demonstrate a twostep functionalization approach for H-terminated boron-doped diamond thin films, which can lead to significant advances in the field of diamond hybrid photovoltaics. Primary diamond surface functionalization is performed via electrochemical diazonium grafting of in situ diazotized 4-iodoaniline. The freshly grafted iodophenyl functional moieties are then employed to couple a layer of thiophene molecules to the diamond surface via two wellestablished Pd-catalyzed cross-coupling reactions, i.e. Stille and Sonogashira. X-ray photoelectron spectroscopy analysis indicates a dense coverage and successful cross-coupling in both cases. However, we find that the Stille reaction is generally accompanied with severe surface contamination, in spite of process optimization and thorough rinsing. Sonogashira cross-coupling on the other hand provides a clean, high quality functionalization over a broad range of reaction conditions. The protocols employing Sonogashira reactions thus appear to be the method of choice toward future fabrication of high-performance dye-functionalized diamond electrodes for photovoltaic applications.