18 Search Results

Abstract The multi‐principal element alloy nanoparticles (MPEA NPs), a new class of nanomaterials, present a highly rewarding opportunity to explore new or vastly different functional properties than the traditional mono/bi/multimetallic nanostructures due to their unique characteristics of atomic‐level homogeneous mixing of constituent elements in the nanoconfinements. Here, the successful creation of NiCoCr nanoparticles, a well‐known MPEA system is reported, using ultrafast nanosecond laser‐induced dewetting of alloy thin films. Nanoparticle formation occurs by spontaneously breaking the energetically unstable thin films in a melt state under laser‐induced hydrodynamic instability and subsequently accumulating in a droplet shape via surface energy minimization. While NiCoCr alloymore » shows a stark contrast in physical properties compared to individual metallic constituents, i.e., Ni, Co, and Cr, yet the transient nature of the laser‐driven process facilitates a homogeneous distribution of the constituents (Ni, Co, and Cr) in the nanoparticles. Using high‐resolution chemical analysis and scanning nanodiffraction, the environmental stability and grain arrangement in the nanoparticles are further investigated. Thermal transport simulations reveal that the ultrashort (≈100 ns) melt‐state lifetime of NiCoCr during the dewetting event helps retain the constituent elements in a single‐phase solid solution with homogenous distribution and opens the pathway to create the unique MPEA nanoparticles with laser‐induced dewetting process.« less

To employ graphene’s rapid conduction in 2D devices, a heterostructure with a broad bandgap dielectric that is free of traps is required. Within this paradigm, h-BN is a good candidate because of its graphene-like structure and ultrawide bandgap. We show how to make such a heterostructure by irradiating alternating layers of a-C and a-BN film with a nanosecond excimer laser, melting and zone-refining constituent layers in the process. With Raman spectroscopy and ToF-SIMS analyses, we demonstrate this localized zone-refining into phase-pure h-BN and rGO films with distinct Raman vibrational modes and SIMS profile flattening after laser irradiation. Furthermore, in comparingmore » laser-irradiated rGO-Si MS and rGO/h-BN/Si MIS diodes, the MIS diodes exhibit an increased turn-on voltage (4.4 V) and low leakage current. The MIS diode I-V characteristics reveal direct tunneling conduction under low bias and Fowler-Nordheim tunneling in the high-voltage regime, turning the MIS diode ON with improved rectification and current flow. This study sheds light on the nonequilibrium approaches to engineering h-BN and graphene heterostructures for ultrathin field effect transistor device development.« less

Er₂Sn₂O₇ pyrochlore was irradiated with swift heavy Au ions (2.2 GeV), and the induced structural modifications were systematically examined using complementary characterization techniques including transmission electron microscopy (TEM), X-ray diffraction (XRD), and neutron total scattering with pair distribution function (PDF) analysis. Each technique probes different aspects and length scales of the transformed material regions. TEM revealed a core–shell ion track structure—an amorphous core surrounded by a disordered, anion-deficient fluorite shell—which was confirmed by XRD. Neutron total scattering, with sensitivity to the oxygen sublattice, provided relative fractions of amorphous and disordered fluorite phases and confirmed the presence of a defective pyrochloremore » phase, which largely maintains its structural ordering but is clearly distinct from the pristine pyrochlore matrix. This defect-rich pyrochlore phase forms a halo extending radially beyond the well-characterized core–shell track morphology observed in electron micrographs. Despite their differing long-range periodicity, the short-range structures of the amorphous, disordered, and defective pyrochlore phases are all modeled well with a weberite-type configuration. Evolution of the phase fractions with increasing ion fluence was examined to ascertain the phase-to-phase pathways that occur during primary and secondary ion impact. Furthermore, this approach extends knowledge about the multi-scale response of stannate pyrochlores to swift heavy ion irradiation in the electronic energy loss regime and improves existing track-overlap models.« less

Abstract Control over the concurrent occurrence of structural (monoclinic to tetragonal) and electrical (insulator to the conductor) transitions presents a formidable challenge for VO ₂ -based thin film devices. Speed, lifetime, and reliability of these devices can be significantly improved by utilizing solely electrical transition while eliminating structural transition. We design a novel strain-stabilized isostructural VO ₂ epitaxial thin-film system where the electrical transition occurs without any observable structural transition. The thin-film heterostructures with a completely relaxed NiO buffer layer have been synthesized allowing complete control over strains in VO ₂ films. The strain trapping in VO ₂ thin filmsmore » occurs below a critical thickness by arresting the formation of misfit dislocations. We discover the structural pinning of the monoclinic phase in (10 ± 1 nm) epitaxial VO ₂ films due to bandgap changes throughout the whole temperature regime as the insulator-to-metal transition occurs. Using density functional theory, we calculate that the strain in monoclinic structure reduces the difference between long and short V-V bond-lengths (Δ _{V − V} ) in monoclinic structures which leads to a systematic decrease in the electronic bandgap of VO ₂ . This decrease in bandgap is additionally attributed to ferromagnetic ordering in the monoclinic phase to facilitate a Mott insulator without going through the structural transition.« less

We report that atomically disordered oxides are seen as suitable candidate for fast oxygen conduction due to their remarkable enhancement in oxygen diffusivity compared with ordered oxides. In particular, disordered derivatives of pyrochlore-structured oxides (A₂B₂O₇) are seen as an interesting prospect due to the intrinsic existence of oxygen vacancies in their lattice. Using energetic ion irradiation, we demonstrated fabrication of structurally disordered nanoscale channels in A₂B₂O₇ (A = Gd, Yb; B = Ti, Zr) that act as selective pathways for fast oxygen conduction. Atomic-level characterization revealed that the amorphous core and surrounding defect-fluorite phase in the nanochannels exhibited distorted andmore » differently coordinated Ti-O polyhedra, with very similar electronic structure. Lastly, the formation of defect-fluorite structure is facilitated by a decrease in the difference between the ionic radii of A- and B-site cations in the lattice.« less

Research efforts in large area graphene synthesis have been focused on increasing grain size. Here, it is shown that, beyond 1 μm grain size, grain boundary engineering determines the electronic properties of the monolayer. It is established by chemical vapor deposition experiments and first-principle calculations that there is a thermodynamic correlation between the vapor phase chemistry and carbon potential at grain boundaries and triple junctions. As a result, boundary formation can be controlled, and well-formed boundaries can be intentionally made defective, reversibly. In 100 µm long channels this aspect is demonstrated by reversibly changing room temperature electronic mobilities from 1000more » to 20,000 cm2 V-1 s-1 . Water permeation experiments show that changes are localized to grain boundaries. Electron microscopy is further used to correlate the global vapor phase conditions and the boundary defect types. Such thermodynamic control is essential to enable consistent growth and control of two-dimensional layer properties over large areas.« less

The formation of metastable phases has attracted significant attention because of their unique properties and potential functionalities. In the present study, we demonstrate the phase conversion of energetic-ion-induced amorphous nanochannels/tracks into a metastable defect fluorite in A₂B₂O₇ structured complex oxides by electron irradiation. Through in situ electron irradiation experiments in a scanning transmission electron microscope, we observe electron-induced epitaxial crystallization of the amorphous nanochannels in Yb₂Ti₂O₇ into the defect fluorite. This energetic-electron-induced phase transformation is attributed to the coupled effect of ionization-induced electronic excitations and local heating, along with subthreshold elastic energy transfers. We also show the role of ionicmore » radii of A-site cations (A = Yb, Gd, and Sm) and B-site cations (Ti and Zr) in facilitating the electron-beam-induced crystallization of the amorphous phase to the defect-fluorite structure. The formation of the defect-fluorite structure is eased by the decrease in the difference between ionic radii of A- and B-site cations in the lattice. Molecular dynamics simulations of thermal annealing of the amorphous phase nanochannels in A₂B₂O₇ draw parallels to the electron-irradiation-induced crystallization and confirm the role of ionic radii in lowering the barrier for crystallization. Furthermore, these results suggest that employing guided electron irradiation with atomic precision is a useful technique for selected area phase formation in nanoscale printed devices.« less

Latent ion tracks created by energetic heavy ions (12 MeV Ti to 946 MeV Au) in single crystal SrTiO₃ are investigated in this paper using Rutherford backscattering spectrometry and scanning transmission electron microscopy. The results demonstrate that pre-existing irradiation damage, introduced via elastic collision processes, interacts synergistically with the electronic energy deposition from energetic heavy ions to enhance formation of latent ion tracks. The average amorphous cross-section increases with the level of pre-damage and is linearly proportional to the electronic energy loss of the ions, with a slope dependent on the pre-damage level. For the highest energy ions (629 MeVmore » Xe and 946 MeV Au), the tracks are continuous over the pre-damaged depth, but become discontinuous beyond the pre-damaged region. Finally, this work provides new understanding and insights on ion-solid interactions that significantly impact the interpretation of latent track formation processes, models of amorphization, and the fabrication of electro-ceramic devices.« less

One of the biggest challenges in the radiation induced defect science is to understand the complex nature of ion-atom interactions under highly extreme conditions. Here, we report the irradiation induced non-equilibrium defect formation in NiCoCr single phase concentrated solid solution alloy due to (i) the extreme inelastic and (ii) the coupled inelastic and elastic ion-atom interactions. These two conditions are achieved at 5 and 30 μm penetration depths along the paths of swift heavy ions (1.542 GeV Bi). In general, the irradiation induced damage consists of interstitial-type dislocation loops and vacancy-type stacking fault tetrahedra (SFT). Near the surface (~5 μm)more » where electronic energy loss is dominating (~62.5 keV nm^–1), the atomic motion primarily results in the formation of SFT. A noticeable increase of dislocation loop formation is observed at 30 μm near the maximum energy deposition from elastic interactions (~4.9 keV nm^–1), as compared to the near surface region (~0.06 keV nm^–1). As a result, insights on the complex electronic and atomic correlations of extreme energy deposition and dissipation on defect dynamics and structural stability may pave the way for new design principles of radiation–tolerant structural alloys.« less

Concentrated solid solution alloys have attracted rapidly increasing attention due to their potential for designing materials with high tolerance to radiation damage. To tackle the effects of chemical complexity in defect dynamics and radiation response, we present in this paper a computational study on swift heavy ion induced effects in Ni and equiatomic Ni -based alloys (Ni₅₀Fe₅₀, Ni₅₀Co₅₀) using two-temperature molecular dynamics simulations (2T-MD). The electronic heat conductivity in the two-temperature equations is parameterized from the results of first principles electronic structure calculations. A bismuth ion (1.542 GeV) is selected and single impact simulations performed in each target. We studymore » the heat flow in the electronic subsystem and show that alloying Ni with Co or Fe reduces the heat dissipation from the impact by the electronic subsystem. Simulation results suggest no melting or residual damage in pure Ni while a cylindrical region melts along the ion propagation path in the alloys. In Ni₅₀Co₅₀ the damage consists of a dislocation loop structure (d = 2 nm) and isolated point defects, while in Ni₅₀Fe₅₀, a defect cluster (d = 4 nm) along the ion path is, in addition, formed. The simulation results are supported by atomic-level structural and defect characterizations in bismuth-irradiated Ni and Ni₅₀Fe₅₀. Finally, the significance of the 2T-MD model is demonstrated by comparing the results to those obtained with an instantaneous energy deposition model without consideration of e-ph interactions in pure Ni and by showing that it leads to a different qualitative behavior.« less