The van der Waals material GeSe is a potential solar absorber, but its optoelectronic properties are not yet fully understood. Here, through a combined theoretical and experimental approach, the optoelectronic and structural properties of GeSe are determined. A fundamental absorption onset of 1.30 eV is found at room temperature, close to the optimum value according to the Shockley–Queisser detailed balance limit, in contrast to previous reports of an indirect fundamental transition of 1.10 eV. The measured absorption spectra and first-principles joint density of states are mutually consistent, both exhibiting an additional distinct onset ∼0.3 eV above the fundamental absorption edge. The band gap values obtained from first-principles calculations converge, as the level of theory and corresponding computational cost increases, to 1.33 eV from the quasiparticle self-consistent GW method, including the solution to the Bethe–Salpeter equation. This agrees with the 0 K value determined from temperature-dependent optical absorption measurements. Relaxed structures based on hybrid functionals reveal a direct fundamental transition in contrast to previous reports. The optoelectronic properties of GeSe are resolved with the system described as a direct semiconductor with a 1.30 eV room temperature band gap. The high level of agreement between experiment and theory encourages the application of this computational methodology to other van der Waals materials.

The physical properties of antimony selenide (Sb 2 Se 3 ) are highly anisotropic. Angle-resolved polarised Raman spectroscopy was employed to characterise oriented crystals and used in conjunction with group theory structural analysis to assign vibrational symmetries to the peaks observed in the Raman spectra.The phonon energies were corroborated via density functional theory (DFT) calculations. Furthermore, a straightforward method is proposed to verify the desirable (001) plane orientation of film growth for device applications via minimisation of the 155 cm À1 peak in the Raman spectrum.

The mussel-inspired properties of dopamine have attracted immense scientific interest for surface modification of nanoparticles due to the high potential of dopamine functional groups to increase the adhesion of nanoparticles to flat surfaces. Here, we report for the first time a novel type of inhibitor-loaded nanocontainer using polydopamine (PDA) as a pH-sensitive gatekeeper for mesoporous silica nanoparticles (MSNs). The encapsulated inhibitor (benzotriazole) was loaded into MSNs at neutral pH, demonstrating fast release in an acidic environment. The self-healing effect of water-borne alkyd coatings doped with nanocontainers was achieved by both on-demand release of benzotriazole during the corrosion process and formation of the complexes between the dopamine functional groups and iron oxides, thus providing dual self-healing protection for the mild steel substrate. The coatings were characterized by electrochemical impedance spectroscopy, visual observations, and confocal Raman microscopy. In all cases, the coatings with embedded benzotriazole-loaded MSNs with PDA-decorated outer surfaces demonstrated superior self-healing effects on the damaged areas. We anticipate that dopamine-based multifunctional gatekeepers can find application potential not only in intelligent self-healing anticorrosive coatings but also in drug delivery, antimicrobial protection, and other fields.

An ever-growing demand for high-energy density and high-power Li-ion batteries has driven active research for electrode materials with superior capacity. Recent years have seen the development of Ni-rich transition metal oxide cathode materials due to their high reversible capacity and lower cost. To achieve full capacity from the charge compensation process, a high voltage (>4.4 V) charging is required. However, the battery operation at higher voltages eventually results in dramatic capacity fading and voltage decay with a rapid decomposition of the electrolyte upon further charge-discharge. While previous studies have reported the degradation mechanism within the electrode surface, there have been few empirical investigations into the solid-electrolyte interphase (SEI) formation on Ni-rich cathodes. In the current work, we visualize the different nature of the electrode-electrolyte interphase at various cut-off voltages (2.0-4.2 V, 2.0-4.5 V, and 2.0-4.8 V). We correlate the key properties of the SEI layer with the capacity fading mechanism in the high capacity battery system. The speciation of transition metal elements (Ni, Mn, and Co) into various oxidation and spin states has been identified as the dominant process of the capacity degradation. Fig. 7 (a) Proposed SEI structures/properties at different cut-off voltages with transition metal spin states, crystal structures, schematics of energy vs. density of states (N(E)) diagram, and visualizations of Li + trapping based on the SIMS profile in the Ni-rich transition metal oxide cathode. (b) Correlation between cut-off voltages, lithium diffusivity (D Li ), SEI impedance (R SEI ), and magnetic moment (m B ).

The improvement of antimony selenide solar cells by shortterm air exposure is explained using complementary cell and material studies. We demonstrate that exposure to air yields a relative efficiency improvement of n-type Sb 2 Se 3 solar cells of ca. 10% by oxidation of the back surface and a reduction in the back contact barrier height (measured by J−V−T) from 320 to 280 meV. X-ray photoelectron spectroscopy (XPS) measurements of the back surface reveal that during 5 days in air, Sb 2 O 3 content at the sample surface increased by 27%, leaving a more Se-rich Sb 2 Se 3 film along with a 4% increase in elemental Se. Conversely, exposure to 5 days of vacuum resulted in a loss of Se from the Sb 2 Se 3 film, which increased the back contact barrier height to 370 meV. Inclusion of a thermally evaporated thin film of Sb 2 O 3 and Se at the back of the Sb 2 Se 3 absorber achieved a peak solar cell efficiency of 5.87%. These results demonstrate the importance of a Se-rich back surface for high-efficiency devices and the positive effects of an ultrathin antimony oxide layer. This study reveals a possible role of back contact etching in exposing a beneficial back surface and provides a route to increasing device efficiency.