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At least 37 records · Page 2

Strain-rate dependent deformation mechanisms in single-layered Cu, Mo, and multilayer Cu/Mo thin films

Here, strain-rate sensitivity and rate-dependent hardness, over a range of 10 -2 to 10 2 s -1 , of sputter-deposited single-layered Cu, Mo, and 5 nm Cu/ 5 nm Mo, and 100 nm Cu/ 100 nm Mo multilayer films with a total film thickness of 5 μm were measured using nanoindentation. The plastic zone underneath the nanoindents was characterized via cross-sectional transmission electron microscopy (XTEM). The multilayer films exhibited enhanced hardness but slightly reduced strain-rate sensitivity with decreasing layer thickness from 100 nm to 5 nm. Only the 5 nm Cu/ 5 nm Mo multilayer film exhibited shear bands underneath the nanoindents, and the size of the shear bands increased with increasing strain rate. In contrast, the 100 nm Cu/ 100 nm Mo multilayer film exhibited material pile-up around the indents and significant nanotwinning within Cu grains. The effect of strain rate and layer thickness on the hardness and strain rate sensitivity of the multilayer thin films is interpreted using a modified confined layer slip (CLS) model. The reduced rate sensitivity at 5 nm as compared to 100 nm correlates with abundant growth nanotwins in the Cu grains in 100 nm and formation of shear bands in 5 nm multilayers. In single layer films, a substructure with a high density of dislocations was observed consistent with the plastic strain gradient in the indent plastic zone. No evidence of deformation twins was noted in any of the samples.

36 MATERIALS SCIENCE↗

Photoluminescence Induced by Substitutional Nitrogen in Single-Layer Tungsten Disulfide

The electronic and optical properties of two-dimensional materials can be strongly influenced by defects, some of which can find significant implementations, such as controllable doping, prolonged valley lifetime, and single-photon emissions. Here, we demonstrate that defects created by remote N 2 plasma exposure in single-layer WS 2 can induce a distinct low-energy photoluminescence (PL) peak at 1.59 eV, which is in sharp contrast to that caused by remote Ar plasma. This PL peak has a critical requirement on the N 2 plasma exposure dose, which is strongest for WS 2 with about 2.0% sulfur deficiencies (including substitutions and vacancies) and vanishes at 5.6% or higher sulfur deficiencies. Both experiments and first-principles calculations suggest that this 1.59 eV PL peak is caused by defects related to the sulfur substitutions by nitrogen, even though low-temperature PL measurements also reveal that not all the sulfur vacancies are remedied by the substitutional nitrogen. The distinct low-energy PL peak suggests that the substitutional nitrogen defect in single-layer WS 2 can potentially serve as an isolated artificial atom for creating single-photon emitters, and its intensity can also be used to monitor the doping concentrations of substitutional nitrogen.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Electrical and Elastic Properties of Individual Single-Layer Nb 4 C 3 T x MXene Flakes

2D carbides and nitrides (MXenes) are widely recognized for their exceptional promise for numerous applications. However, physical property measurements of their individual monolayers remain very limited despite their importance for revealing the intrinsic physical properties of MXenes. The first mechanical and electrical measurements of individual single-layer flakes of Nb 4 C 3 T x MXene, which are prepared via an improved synthetic method are reported. Characterization of field-effect transistor devices based on individual single-layer Nb 4 C 3 T x flakes shows an electrical conductivity of 1024 ± 165 S cm -1 , which is two orders of magnitude higher than the previously reported values for bulk Nb 4 C 3 T x assemblies, and an electron mobility of 0.41 ± 0.27 cm 2 V -1 s -1 . Atomic force microscopy nanoindentation measurements of monolayer Nb 4 C 3 T x membranes yield an effective Young's modulus of 386 ± 13 GPa, assuming a membrane thickness of 1.26 nm. This is the highest value reported for nanoindentation measurements of solution-processable 2D materials, revealing the potential of Nb 4 C 3 T x as a primary component for various mechanical applications. In conclusion, the agreement between the mechanical properties of 2D Nb 4 C 3 T x MXene and cubic NbC suggests that the extensive experimental data on bulk carbides could be useful for identifying new MXenes with improved functional characteristics.

36 MATERIALS SCIENCE↗

Quantification of defects engineered in single layer MoS 2

Atomic defects are controllably introduced in suspended single layer molybdenum disulfide (1L MoS 2 ) using helium ion beam. Vacancies exhibit one missing atom of molybdenum and a few atoms of sulfur. Quantification was done using a Scanning Transmission Electron Microscope (STEM) with an annular detector. Experimentally accessible inter-defect distance was employed to measure the degree of crystallinity in 1L MoS 2 . A correlation between the appearance of an acoustic phonon mode in the Raman spectra and the inter-defect distance was established, which introduces a new methodology for quantifying defects in two-dimensional materials such as MoS 2 .

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Manipulation of Exciton Dynamics in Single-Layer WSe 2 Using a Toroidal Dielectric Metasurface

Recent advances in emerging atomically thin transition metal dichalcogenide semiconductors with strong light–matter interactions and tunable optical properties provide novel approaches for realizing new material functionalities. Coupling two-dimensional semiconductors with all-dielectric resonant nanostructures represents an especially attractive opportunity for manipulating optical properties in both the near-field and far-field regimes. In this work, by integrating single-layer WSe 2 and titanium oxide (TiO 2 ) dielectric metasurfaces with toroidal resonances, we realized robust exciton emission enhancement over 1 order of magnitude at both room and low temperatures. Furthermore, we could control exciton dynamics and annihilation by using temperature to tailor the spectral overlap of excitonic and toroidal resonances, allowing us to selectively enhance the Purcell effect. Our results provide rich physical insight into the strong light–matter interactions in single-layer TMDs coupled with toroidal dielectric metasurfaces, with important implications for optoelectronics and photonics applications.

36 MATERIALS SCIENCE↗

High accuracy single-layer free-space diffractive neuromorphic classifiers for spatially incoherent light

Free-space all-optical diffractive systems have shown promise for neuromorphic classification of objects without converting light to the electronic domain. While the factors that govern these systems have been studied for coherent light, the fundamental properties for incoherent light have not been addressed, despite the importance for many applications. Here we use a co-design approach to show that optimized systems for spatially incoherent light can achieve performance on par with the best linear electronic classifiers even with a single layer containing few diffractive features. This performance is limited by the inherent linear nature of incoherent optical detection. We circumvent this limit by using a differential detection scheme that achieves greater than 94% classification accuracy on the MNIST dataset and greater than 85% classification accuracy for Fashion-MNIST, using a single layer metamaterial.

Léonard, François (ORCID:0000000249736743)↗

Atomic-scale electronic inhomogeneity in single-layer iron chalcogenide alloys revealed by machine learning of STM/S data

Chemical pressure from the isovalent substitution of Se by a larger Te atom in the epitaxial film of iron chalcogenide FeSe can effectively tune its superconducting, topological, and magnetic properties. However, such substitution during epitaxial growth inherently leads to defects and structural inhomogeneity, making the determination of alloy composition and atomic sites for the substitutional Te atoms challenging. Here, we utilize machine learning to distinguish between Se and Te atoms in scanning tunneling microscopy images of single-layer FeSe1−xTex on SrTiO3(001) substrates. Defect locations are first identified by analyzing spatial-dependent dI/dV tunneling spectra using the K-means clustering method. After excluding the defect regions, the remaining dI/dV spectra are further analyzed using the singular value decomposition method to determine the Se/Te ratio. Our findings demonstrate an effective and reliable approach for determining alloy composition and atomic-scale electronic inhomogeneity in superconducting single-layer iron chalcogenide films.

Materials Science↗

Evidence for quantum spin liquid behaviour in single-layer 1T-TaSe 2 from scanning tunnelling microscopy

Two-dimensional triangular-lattice antiferromagnets are predicted under some conditions to exhibit a quantum spin liquid ground state with no energy barrier to create emergent, fractionalized spinon excitations that carry spin but no charge. Materials that realize this kind of spin liquid are expected to have a low-energy behaviour described by a spinon Fermi surface. Directly imaging the resulting spinons, however, is difficult due to their chargeless nature. In this work, we use scanning tunnelling spectroscopy to image density waves consistent with the predictions of spinon density modulation arising from a spinon Fermi surface instability in single-layer 1T-TaSe 2 . We confirm the existence of a triangular lattice of localized spins in this material by contacting it with a metallic 1H-TaSe 2 substrate and measuring the Kondo effect. Spectroscopic imaging of isolated single-layer 1T-TaSe 2 reveals long-wavelength super-modulations at Hubbard band energies, consistent with the predicted behaviour of itinerant spinons. These super-modulations allow the direct experimental measurement of the spinon Fermi wavevector, in good agreement with theoretical predictions for a two-dimensional quantum spin liquid.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗

Phase diagrams of single-layer two-dimensional transition metal dichalcogenides: Landau theory

We report single layer (SL) two-dimensional transition metal dichalcogenides (TMDs), such as MoS 2 , ReS 2 , WSe 2 , and MoTe 2 have now become the focus of intensive fundamental and applied research due to their intriguing and tunable physical properties. These materials exhibit a broad range of structural phases that can be induced via elastic strain, chemical doping, and electrostatic field effect. These transformations, in turn, can open and close the band gap of SL-TMDs, leading to metal-insulator transitions, and lead to emergence of more complex quantum phenomena. These considerations necessitate detailed understanding of the mesoscopic mechanisms of these structural phase transitions. Here we develop a Landau-type thermodynamic description of SL-TMDs on a sample of the SL-(MoS 2 ) 1-x -(ReS 2 ) x system and analyze the free energy surfaces, phase diagrams, and order parameter behavior. Our results predict the existence of multiple structural phases with two-, six- and 12-fold degenerated energy minima for in-plane and out-of-plane order parameters. This analysis suggests that out-of-plane ferroelectricity can exist in many of these phases, with the switchable polarization being proportional to the out-of-plane order parameter. We further predict that the domain walls in SL-(MoS 2 ) 1-x -(ReS 2 ) x should become conductive above a certain strain threshold.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗

Nanoscale friction of CVD single-layer MoS 2 with controlled defect formation

Two-dimensional (2D) layered nanomaterials such as graphene, molybdenum disulfide (MoS 2 ), or tungsten disulfide offer a promising solution in areas of solid-state lubrication, due to their excellent mechanical properties as well as low friction. However, defects can influence their friction and reduce their superior tribological properties. Thus, it is crucial to understand the effects of defects on sliding behavior in 2D nanomaterials, to foster a functional strategy for utilizing 2D nanomaterials as solid-state tribological films. In this study, frictional effects of defects, grain boundaries, and atomic-scale structural defects were explored on chemical vapor deposition (CVD) grown single layer MoS 2 . Selective patterning of defects into MoS 2 was accomplished via controlled irradiation of helium ions with varying ion doses. The friction of MoS 2 was characterized by friction force microscopy (FFM) and was found that friction depends on the defect formation controlled by helium ion irradiation. This approach offers a correlation between surface topography, defects and friction. Understanding the relative friction of MoS 2 in the presence of different levels of defects is foundational to studying tribological properties of a single layer MoS 2 at both nanoscales and macroscales.

36 MATERIALS SCIENCE↗

Exploring few and single layer CrPS 4 with near-field infrared spectroscopy

Abstract We combine synchrotron-based near-field infrared spectroscopy and first principles lattice dynamics calculations to explore the vibrational response of CrPS 4 in bulk, few-, and single-layer form. Analysis of the mode pattern reveals a C 2 polar + chiral space group, no symmetry crossover as a function of layer number, and a series of non-monotonic frequency shifts in which modes with significant intralayer character harden on approach to the ultra-thin limit whereas those containing interlayer motion or more complicated displacement patterns soften and show inflection points or steps. This is different from MnPS 3 where phonons shift as 1/size 2 and are sensitive to the three-fold rotation about the metal center that drives the symmetry crossover. We discuss these differences as well as implications for properties such as electric polarization in terms of presence or absence of the P–P dimer and other aspects of local structure, sheet density, and size of the van der Waals gap.

36 MATERIALS SCIENCE↗

Domain state exchange bias in a single layer FeRh thin film formed via low energy ion implantation

Modern spintronics relies heavily on the exchange bias effect to pin the orientation of ferromagnetic layers in magnetic tunnel junctions. The current implementations of exchange bias in magnetic tunnel junctions employ pristine interfaces between antiferromagnetic and ferromagnetic layers. Here we reveal an interfacial exchange bias introduced by a single-step, low-energy ion implantation process in a single layer FeRh thin film. Both 1 keV He + ions and 5 keV Fe + were investigated, their energy selected to ensure the ions would stop within the FeRh film. The ions reduce the metamagnetic transition temperature through defect generation to form a surface layer with ferromagnetic ordering. Temperature dependent magnetism measurements reveal a room temperature exchange bias between the ferromagnetic surface and the antiferromagnetic bulk of ~41 Oe in 5 keV Fe + implanted samples and ~36 Oe for 1 keV He + implanted samples. We directly scrutinize this exchange bias effect in magnetic depth profiles obtained by polarized neutron reflectometry which clearly show a pinned ferromagnetic layer adjacent to the disordered layer created by low energy Fe + ion implantation. These results reveal a novel method to implement exchange bias in an antiferromagnetic layer that can have direct application in the field of spintronics.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Electronic properties of single-layer CoO 2 /Au(111)

Here we report direct measurements via angle-resolved photoemission spectroscopy (ARPES) of the electronic dispersion of single-layer (SL) CoO 2 . The Fermi contour consists of a large hole pocket centered at the $\overline{\Gamma}$ point. To interpret the ARPES results, we use density functional theory (DFT) in combination with the multi-orbital Gutzwiller Approximation (DFT+GA), basing our calculations on crystalline structure parameters derived from x-ray photoelectron diffraction and low-energy electron diffraction. Our calculations are in good agreement with the measured dispersion. We conclude that the material is a moderately correlated metal. We also discuss substrate effects, and the influence of hydroxylation on the CoO 2 SL electronic structure.

36 MATERIALS SCIENCE↗

Correlations between electronic order and structural distortions and their ultrafast dynamics in the single-layer manganite P r 0.5 C a 1.5 Mn O 4

Time-resolved x-ray diffraction experiments on the half-doped single-layered manganite Pr 0.5 Ca 1.5 Mn O 4 are used to monitor the ultrafast photoinduced dynamics of the structural distortion associated with the charge and orbital ordering (CO/OO). As in the nonlayered three-dimensional counterpart, the ordered phase melts in less than 100 fs after 800-nm photoexcitation and subsequently partially recovers due to thermal equilibration of electronic and vibrational systems. Photoexciting Pr 0.5 Ca 1.5 Mn O 4 below the transition temperature of a second structural phase transition that occurs around 146 K (deep inside the CO/OO phase) releases this structural transition, but progresses on a much slower timescale. Finally, this additional reduction of crystal symmetry, which we ascribe to a further tilt of the oxygen octahedra, can thus be considered to be only weakly coupled to CO/OO. Furthermore, static hard-x-ray and resonant soft-x-ray diffraction at the Mn L 2,3 edges experiments identify correlations between structural distortions and electronic order in thermal equilibrium.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗

Single-Layer Dititanium Oxide Ti 2 O MOene: Multifunctional Promises for Electride, Anode Materials, and Superconductor

Using the first-principles calculations, we report the existence of the single-layer (SL) dititanium oxide Ti 2 O (labeled as MOene) that constructs a novel family of MXene based on transition-metal oxides. This MOene material strongly contrasts the conventional ones consisting of transition-metal carbides and/or nitrides. SL Ti 2 O has high thermal and dynamical stabilities because of the strong Ti–O ionic bonding interactions. Moreover, this material is an intrinsic electride and exhibits extremely low diffusion barriers of ~12.0 and 6.3 meV for Li and Na diffusion, respectively. When applied as anode materials in lithium-ion batteries and sodium-ion batteries, it possesses a high energy storage capacity (960.23 mAhg –1 ), surpassing the traditional MXenes-based anodes. The superb electrochemical performance stems from the existing anionic electron on Ti 2 O surface. Astonishingly, SL Ti 2 O is also determined to be a superconductor with a superconducting transition temperature (T c ) of ~9.8 K, which originates from the soft-mode of the first acoustic phonon branch and enhanced electron–phonon coupling in the low-frequency region. Furthermore, this soft-mode behaves much softer upon applying a compressive strain of 2%, leading to a higher T c of 11.9 K. Furthermore, our finding broadens the family of MXenes and could facilitate more experimental efforts toward future nanodevices.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Pt Atomic Single-Layer Catalyst Embedded in Defect-Enriched Ceria for Efficient CO Oxidation

The local coordination structure of metal sites essentially determines the performance of supported metal catalysts. Here, using a surface defect enrichment strategy, we successfully fabricated Pt atomic single-layer (Pt ASL ) structures with 100% metal dispersion and precisely controlled local coordination environment (embedded vs adsorbed) derived from Pt single-atoms (Pt 1 ) on ceria-alumina supports. The local coordination environment of Pt 1 not only governs its catalytic activity but also determines the Pt 1 structure evolution upon reduction activation. For CO oxidation, the highest turnover frequency can be achieved on the embedded Pt ASL in the CeO 2 lattice, which is 3.5 times of that on the adsorbed Pt ASL on the CeO 2 surface and 10–70 times of that on Pt1. The favorable CO adsorption on embedded Pt ASL and improved activation/reactivity of lattice oxygen within CeO 2 effectively facilitate the CO oxidation. This work provides new insights for the precise control of the local coordination structure of active metal sites for achieving 100% atomic utilization efficiency and optimal intrinsic catalytic activity for targeted reactions simultaneously.

36 MATERIALS SCIENCE↗

Landscape of coexisting excitonic states in the insulating single-layer cuprates and nickelates

We present an ab initio study of the excitonic states of a prototypical high-temperature superconductor La 2 CuO 4 and compare them to the isostructural single-layer nickelate La 2 NiO 4 . A key difference in the low-energy electronic structure leads to very different excitonic behavior. Excitons in La 2 CuO 4 are delocalized and can freely move in the CuO 2 plane without disturbing the antiferromagnetic order. In contrast, in La 2 NiO 4 , we find the low-lying excitonic states to be extremely localized, producing a nearly flat dispersion. The theoretically obtained excitonic dispersion and behavior are in excellent agreement with RIXS observations. To classify the excitons, we project the electron-hole coupling onto each atomic site including the full manifold of atomic orbitals. We find the excitons to be composed of a linear combination of exciton classes, including Mott-Hubbard, d-d, and charge-transfer. The implication of these excitations to the high-T c pairing mechanism is also discussed.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗

Permeability of Single–Layer–Free–Standing Meshes at Varying Capillary Pressure via a Novel Method

The permeability of mesh wicks is important for various applications, including two–phase heat transfer. However, the understanding of the permeability of single–layer, free–standing mesh wicks, with liquid–gas interfaces on both sides, is limited. A novel and simpler method is presented to determine the permeability of a free–standing wick and apply it to a representative mesh. This method involves modifying the capillary pressure via elevation and simultaneously measuring the permeability to determine the permeability–capillary pressure relationship. When applied to a copper mesh with plain weave having undergone surface cleaning, the permeability is found to decrease as capillary pressure for deionized water increases. A dimensional analysis is presented to generalize this data for other mesh sizes with similar weaves and fluids. The behavior of mesh in application is modeled, based on the integration of Darcy's law with an analytic function fit to measured data, and parametric studies are conducted to investigate the superficial velocity of liquids through the mesh under varying driving pressures, transport lengths, and liquid viscosity, based on the obtained capillary pressure–permeability relationship. This study provides valuable insights into the transport properties of mesh wicks, with potential applications in fields such as electronics cooling, electrochemical devices, and fluid purification technologies.

36 MATERIALS SCIENCE↗