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Register a new userElectronic excitation of transition metal nitrides by light ions with keV energies
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We investigated the specific electronic energy deposition by protons and He ions with keV energies in different transition metal nitrides of technological interest. Data were obtained from two different time-of-flight ion scattering setups and show excellent agreement. For protons interacting with light nitrides, i.e. TiN, VN and CrN, very similar stopping cross sections per atom were found, which coincide with literature data of N2 gas for primary energies <= 25 keV. In case of the chemically rather similar nitrides with metal constituents from the 5th and 6th period, i.e. ZrN and HfN, the electronic stopping cross sections were measured to exceed what has been observed for molecular N2 gas. For He ions, electronic energy loss in all nitrides was found to be significantly higher compared to the equivalent data of N2 gas. Additionally, deviations from velocity proportionality of the observed specific electronic energy loss are observed. A comparison with predictions from density functional theory for protons and He ions yields a high apparent efficiency of electronic excitations of the target for the latter projectile. These findings are considered to indicate the contributions of additional mechanisms besides electron hole pair excitations, such as electron capture and loss processes of the projectile or promotion of target electrons in atomic collisions.
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Extraction of non-equilibrium hot carriers generated by plasmon decay in metallic nanostructures is an increasingly exciting prospect for utilizing plasmonic losses, but the search for optimum plasmonic materials with long-lived carriers is ongoing. Transition metal nitrides are an exciting class of new plasmonic materials with superior thermal and mechanical properties compared to conventional noble metals, but their suitability for plasmonic hot carrier applications remains unknown. Here, we present fully first-principles calculations of the plasmonic response, hot carrier generation and subsequent thermalization of all group IV, V and VI transition metal nitrides, fully accounting for direct and phonon-assisted transitions as well as electron-electron and electron-phonon scattering. We find the largest frequency ranges for plasmonic response in ZrN, HfN and WN, between those of gold and silver, while we predict strongest absorption in the visible spectrum for the VN, NbN and TaN. Hot carrier generation is dominated by direct transitions for most of the relevant energy range in all these nitrides, while phonon-assisted processes dominate only below 1 eV plasmon energies primarily for the group IV nitrides. Finally, we predict the maximum hot carrier lifetimes to be around 10 fs for group IV and VI nitrides, a factor of 3 - 4 smaller than noble metals, due to strong electron-phonon scattering. However, we find longer carrier lifetimes for group V nitrides, comparable to silver for NbN and TaN, while exceeding 100 fs (twice that of silver) for VN, making them promising candidates for efficient hot carrier extraction.
Graphene is expected to be rather insensitive to ionizing particle radiation. We demonstrate that single layers of exfoliated graphene sustain significant damage from irradiation with slow highly charged ions. We have investigated the ion induced changes of graphene after irradiation with highly charged ions of different charge states (q = 28-42) and kinetic energies E_kin = 150-450 keV. Atomic force microscopy images reveal that the ion induced defects are not topographic in nature but are related to a significant change in friction. To create these defects, a minimum charge state is needed. In addition to this threshold behaviour, the required minimum charge state as well as the defect diameter show a strong dependency on the kinetic energy of the projectiles. From the linear dependency of the defect diameter on the projectile velocity we infer that electronic excitations triggered by the incoming ion in the above-surface phase play a dominant role for this unexpected defect creation in graphene.
Metal-ion doping can effectively regulate the metal-insulator transition temperature in $mathrm{VO}_2$. Experiments found that the pentavalent and hexavalent ion doping dramatically reduces the transition temperature while the trivalent ion doping increases the transition temperature and induces intermediate phases. Based on the phase-field model of the metal-insulator transition in $mathrm{VO}_2$ we developed previously, we formulate a Landau potential of the metal-ion-doped $mathrm{VO}_2$ taking account of the effects of doping on the electron correlation and lattice structure. The effect of metal-ion doping on the lattice structure is accounted for in a phenomenological way. Using the Landau potential, we calculate the temperature-dopant-concentration phase diagrams of $mathrm{VO}_2$ doped with various metal ions consistent with the experiments and provide explanation to the different behaviors of different metal-ion doping. The phenomenological theory can provide estimations of phase diagrams of $mathrm{VO}_2$ doped with other metal ions.
Energy spectra of backscattered and transmitted ions with primary energies of 50 keV and 100 keV interacting with self-supporting foils were recorded with a Time-of-Flight Medium-Energy Ion Scattering setup in a single experiment. Self-supporting Au and W foils without backing material were used. For He ions transmitted through Au the spectrum of detected particles shows two distinct components corresponding to different energy losses in the film, whereas for protons no such phenomenon was observed. To determine the origin of these different contributions, measurements for different angles of incidence and scattering angles have been evaluated. The results suggest that the two components in the spectrum of transmitted He ions could be attributed to impact parameter dependent energy loss, being more prominent for He ions than for protons. The main origin of the necessary impact parameter selection along the different ion trajectories is expected to be texture in the Au-foils.
Modulating electronic structure of monolayer transition metal dichalcogenides (TMDCs) is important for many applications and doping is an effective way towards this goal, yet is challenging to control. Here we report the in-situ substitutional doping of niobium (Nb) into TMDCs with tunable concentrations during chemical vapour deposition. Taking monolayer WS2 as an example, doping Nb into its lattice leads to bandgap changes in the range 1.98 eV to 1.65 eV. Noteworthy, electrical transport measurements and density functional theory calculations show that the 4d electron orbitals of the Nb dopants contribute to the density of states of Nb-doped WS2 around the Fermi level, resulting in an n to p-type conversion. Nb-doping also reduces the energy barrier of hydrogen absorption in WS2, leading to an improved electrocatalytic hydrogen evolution performance. These results highlight the effectiveness of controlled doping in modulating the electronic structure of TMDCs and their use in electronic related applications.
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