Unraveling the Role of Orbital Interaction in the Electrochemical HER of the Trimetallic AgAuCu Nanobowl Catalyst.

Unraveling the origins of the electrocatalytic activity of composite nanomaterials is crucial but inherently challenging. Here, we present a comprehensive investigation of the influence of different orbitals' interaction in the AuAgCu nanobowl model electrocatalyst during the hydrogen evolution reaction (HER). According to our theoretical study, AgAuCu exhibits a lower energy barrier than AgAu and AgCu bimetallic systems for the HER, suggesting that the trimetallic AgAuCu system interacts optimally with H*, resulting in the most efficient HER catalyst. As we delve deeper into the HER activity of AgAuCu, it was observed that the presence of Cu allows Au to adsorb the H* intermediate through the hybridization of s orbitals of hydrogen and s, dx2-y2, and dz2 orbitals of Au. Such orbital interaction was not present in the cases of AgAu and AgCu bimetallic systems, and as a result, these bimetallic systems exhibit lower HER activities.

Electronic Structure and Enhanced Charge-Density Wave Order of Monolayer VSe2.

How the interacting electronic states and phases of layered transition-metal dichalcogenides evolve when thinned to the single-layer limit is a key open question in the study of two-dimensional materials. Here, we use angle-resolved photoemission to investigate the electronic structure of monolayer VSe2 grown on bilayer graphene/SiC. While the global electronic structure is similar to that of bulk VSe2, we show that, for the monolayer, pronounced energy gaps develop over the entire Fermi surface with decreasing temperature below Tc = 140 ± 5 K, concomitant with the emergence of charge-order superstructures evident in low-energy electron diffraction. These observations point to a charge-density wave instability in the monolayer that is strongly enhanced over that of the bulk. Moreover, our measurements of both the electronic structure and of X-ray magnetic circular dichroism reveal no signatures of a ferromagnetic ordering, in contrast to the results of a recent experimental study as well as expectations from density functional theory. Our study thus points to a delicate balance that can be realized between competing interacting states and phases in monolayer transition-metal dichalcogenides.

Signatures of the Kondo effect in VSe2.

VSe2 is a transition metal dichaclogenide which has a charge- density wave transition that has been well studied. We report on a low-temperature upturn in the resistivity and, at temperatures below this resistivity minimum, an unusual magnetoresistance which is negative at low fields and positive at higher fields, in single crystals of VSe2. The negative magnetoresistance has a parabolic dependence on the magnetic field and shows little angular dependence. The magnetoresistance at temperatures above the resistivity minimum is always positive. We interpret these results as signatures of the Kondo effect in VSe2. An upturn in the susceptibility indicates the presence of interlayer V ions which can provide the localized magnetic moments required for scattering the conduction electrons in the Kondo effect. The low-temperature behaviour of the heat capacity, including a high value of γ, along with a deviation from a Curie-Weiss law observed in the low-temperature magnetic susceptibility, are consistent with the presence of magnetic interactions between the paramagnetic interlayer V ions and a Kondo screening of these V moments.

Evidence for topological surface states in metallic single crystals of Bi2Te3.

Bi2Te3 is a member of a new class of materials known as topological insulators which are supposed to be insulating in the interior and conducting on the surface. However, experimental verification of the conductive qualities of the surface states has been hindered by parallel bulk conductions. We report low temperature magnetotransport measurements on single crystal samples of Bi2Te3. We observe metallic character in our samples and large and linear magnetoresistance from 1.5 K to 290 K with prominent Shubnikov-de Haas (SdH) oscillations whose traces persist up to 20 K. Even though our samples are metallic, we are able to obtain a Berry phase close to the value of π, which is expected for Dirac fermions of the topological surface states. This indicates that we have obtained evidence for the topological surface states in metallic single crystals of Bi2Te3. Other physical measurements obtained from the analysis of the SdH oscillations are also in close agreement with those reported for the topological surface states. The linear magnetoresistance observed in our sample, which is considered as a signature of the Dirac fermions of the surface states, lends further credence to the existence of topological surface states.