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Crystal plasticity modeling for the strengthening effect of multilayered copper–graphene nanocomposites
The paper explores plastic deformation mechanisms in metal–graphene nanocomposites, illustrating their material strengthening effects through a crystal plasticity finite element (CPFE) model. This model is compared with published experimental results, which have previously shown that the two-dimensional shape of graphene effectively controls dislocation motion and significantly enhances the strength of metals. Simulated nanopillar compression tests, using a physics-based CP model that incorporates surface nucleation and single-arm source dislocation mechanisms, help us understand dislocation motions at submicron length scales. The crystal plasticity models are applied to nanolayered composites with copper grain layers and monolayer graphene, featuring repeat layer spacings of 200 nm, 125 nm, and 70 nm, respectively. This study quantifies the accumulation of dislocations at the graphene interfaces, contributing to the ultra-high strength of copper–graphene composites. Furthermore, a Hall–Petch-like correlation is established between yield strength and the number of embedded graphene layers.
Surface Termination Dependent Work Function and Electronic Properties of Ti 3 C 2 T x MXene
MXenes, an emerging family of 2D transition metal carbides and nitrides, have shown promise in various applications, such as energy storage, electromagnetic interference shielding, conductive thin films, photonics, and photothermal therapy. Their metallic nature, wide range of optical absorption, and tunable surface chemistry are the key to their success in those applications. The physical properties of MXenes are known to be strongly dependent on their surface terminations. In this study, we investigated the electronic properties of Ti 3 C 2 T x for different surface terminations, as achieved by different annealing temperatures, with the help of photoelectron spectroscopy, inverse photoelectron spectroscopy, and density functional theory calculations. We find that fluorine occupies solely the face-centered cubic adsorption site, whereas oxygen initially occupies at least two different adsorption sites, followed by a rearrangement after fluorine desorption at high annealing temperatures. The measured electronic structure of Ti 3 C 2 T x showed strong dispersion of more than 1 eV, which we conclude to stem from Ti–O bonds by comparing it to calculated band structures. We further measured the work function of Ti 3 C 2 T x as a function of annealing temperature and found that it is in the range of 3.9–4.8 eV, depending on the surface composition. A comparison of the experimental work function to detailed density functional theory calculations shows that the measured value is not simply an average of the work function values of uniformly terminated Ti 3 C 2 surfaces but that the interplay between the different surface moieties and their local dipoles plays a crucial role.
Atomic-Scale Imprinting by Sputter Deposition of Amorphous Metallic Films
Not Available
Tuning the Chern number in quantum anomalous Hall insulators
A quantum anomalous Hall (QAH) state is a two-dimensional topological insulating state that has a quantized Hall resistance of h/(Ce 2 ) and vanishing longitudinal resistance under zero magnetic field (where h is the Planck constant, e is the elementary charge, and the Chern number C is an integer). The QAH effect has been realized in magnetic topological insulators and magic-angle twisted bilayer graphene. However, the QAH effect at zero magnetic field has so far been realized only for C = 1. Here we realize a well quantized QAH effect with tunable Chern number (up to C = 5) in multilayer structures consisting of alternating magnetic and undoped topological insulator layers, fabricated using molecular beam epitaxy. The Chern number of these QAH insulators is determined by the number of undoped topological insulator layers in the multilayer structure. Moreover, we demonstrate that the Chern number of a given multilayer structure can be tuned by varying either the magnetic doping concentration in the magnetic topological insulator layers or the thickness of the interior magnetic topological insulator layer. We develop a theoretical model to explain our experimental observations and establish phase diagrams for QAH insulators with high, tunable Chern number. Furthermore, the realization of such insulators facilitates the application of dissipationless chiral edge currents in energy-efficient electronic devices, and opens up opportunities for developing multi-channel quantum computing and higher-capacity chiral circuit interconnects.
Machine learning prediction of connectivity, biodiversity and resilience in the Coral Triangle
Abstract Even optimistic climate scenarios predict catastrophic consequences for coral reef ecosystems by 2100. Understanding how reef connectivity, biodiversity and resilience are shaped by climate variability would improve chances to establish sustainable management practices. In this regard, ecoregionalization and connectivity are pivotal to designating effective marine protected areas. Here, machine learning algorithms and physical intuition are applied to sea surface temperature anomaly data over a twenty-four-year period to extract ecoregions and assess connectivity and bleaching recovery potential in the Coral Triangle and surrounding oceans. Furthermore, the impacts of the El Niño Southern Oscillation (ENSO) on biodiversity and resilience are quantified. We find that resilience is higher for reefs north of the Equator and that the extraordinary biodiversity of the Coral Triangle is dynamic in time and space, and benefits from ENSO. The large-scale exchange of genetic material is enhanced between the Indian Ocean and the Coral Triangle during La Niña years, and between the Coral Triangle and the central Pacific in neutral conditions. Through machine learning the outstanding biodiversity of the Coral Triangle, its evolution and the increase of species richness are contextualized through geological times, while offering new hope for monitoring its future.
Synchrotron-based ambient pressure X-ray photoelectron spectroscopy of hydrogen and helium
Contrary to popular belief, it is possible to obtain X-ray photoelectron spectra for elements lighter than lithium, namely hydrogen and helium. The literature is plagued with claims of this impossibility, which holds true for lab-based X-ray sources. However, this limitation is merely technical and is related mostly to the low X-ray photoionization cross-sections of the 1s orbitals of hydrogen and helium. Here, we show that, using ambient pressure X-ray photoelectron spectroscopy (XPS), a bright-enough X-ray source allows the study of these elusive elements. This has important implications in the understanding of the limitations of one of the most useful techniques in materials science, and moreover, it potentially opens the possibility of using XPS to directly study the most abundant element in the universe.
Direct synthesis of biaxially textured nickel disilicide thin films by magnetron sputter deposition on low-cost metal tapes for flexible silicon devices
Nickel silicides are widely used as contact materials for electronic devices based on silicon (Si). However, they have been predominantly fabricated by annealing separate Ni and Si phases which leads to phase and structural complexity. In this letter, direct epitaxial growth of a single-phase nickel disilicide (NiSi 2 ) thin film by sputter deposition of NiSi 2 is achieved on low-cost and flexible Hastelloy tapes which offers a promising route to fabricate low-cost, flexible electronic devices. Biaxially textured titanium nitride (TiN) is applied as the seeding layer and the diffusion barrier under NiSi 2 . An epitaxial relationship of (001)$\langle$100$\rangle$NiSi 2 ∥ (001)$\langle$110$\rangle$TiN is observed with an extra-large lattice mismatch (~10.3%) between NiSi 2 and TiN. Both the bonding similarity and the passivation effect by hydrogen promote the epitaxial growth of NiSi 2 on TiN. The flat and smooth NiSi 2 thin film consists of grains with a size of 50–100 nm. An epitaxially grown Si film on NiSi 2 further demonstrates the potential of manufacturing high-performance Si flexible electronics with NiSi 2 /TiN/Hastelloy as the direct contact through this approach.
Dynamically weighted multireference perturbation theory: Combining the advantages of multi-state and state-averaged methods
In this paper, we introduce two new approaches to compute near-degenerate electronic states based on the driven similarity renormalization group (DSRG) framework. The first approach is a unitary multi-state formalism based on the DSRG (MS-DSRG), whereby an effective Hamiltonian is built from a set of state-specific solutions. The second approach employs a dynamic weighting parameter to smoothly interpolate between the multi-state and the state-averaged DSRG schemes. The resulting dynamically weighted DSRG (DW-DSRG) theory incorporates the most desirable features of both multi-state approaches (ability to accurately treat many states) and state-averaged methods (correct description of avoided crossings and conical intersections). We formulate second-order perturbation theories (PT2) based on the MS- and DW-DSRG and study the potential energy curves of LiF, the conical intersection of the two lowest singlet states of NH 3 , and several low-lying excited states of benzene, naphthalene, and anthracene. The DW-DSRG-PT2 predicts the correct avoided crossing of LiF and avoids artifacts produced by the corresponding state-specific and multi-state theories. Excitation energies of the acenes computed with the DW-DSRG-PT2 are found to be more accurate than the corresponding state-averaged values, showing a small dependence on the number of states computed.
Analytic gradients for the single-reference driven similarity renormalization group second-order perturbation theory
Herein we derive and implement analytic energy gradients for the single-reference driven similarity renormalization group second-order perturbation theory (DSRG-PT2). The resulting equations possess an asymptotic scaling that is identical to that of the second-order Møller–Plesset perturbation theory (MP2), indicating that the exponential regularizer in the DSRG equations does not introduce formal difficulties in the gradient theory. We apply the DSRG-PT2 method to optimizing the geometries of 15 small molecules. The equilibrium bond lengths computed with DSRG-PT2 are found similar to those of MP2, yielding a mean absolute error of 0.0033 Å and a standard deviation of 0.0045 Å when compared with coupled cluster with singles, doubles, and perturbative triples.
Strong-field coherence breaking as a tool for identifying methyl rotor states in microwave spectra: 2-hexanone
The rotational spectrum of 2-hexanone was recorded over the 8–18 GHz region using a chirped pulse Fourier transform microwave spectrometer. Strong field coherence breaking (SFCB) was utilized to selectively modulate the intensities of rotational transitions belonging to the two lowest energy conformers of 2-hexanone, aiding the assignment. In addition, the SFCB method was applied for the first time to selectively identify rotational transitions built off the two lowest energy hindered methyl rotor states of each conformer, 0a1 and 1e. Since these two states have rotational energy levels with different nuclear spin symmetries, their intensities could be selectively modulated by the resonant monochromatic pulses used in the SFCB method. Here, the difference spectra, final fit, and structural parameters are discussed for the three assigned conformers of 2-hexanone.
Adaptive strong-field control of vibrational population in NO 2+
An adaptive closed-loop system employing coincidence time-of-flight feedback is used to determine the optimal pulse shapes for manipulating the branching ratio of NO dications following double ionization by an intense laser pulse. Selection between the long-lived NO 2+ and the dissociative N + + O + final states requires control of the vibrational population distribution in the transient NO 2+ . The ability to both suppress and enhance NO 2+ relative to N + + O + is observed, with the effectiveness of shaped pulses surpassing near Fourier transform-limited pulses by about an order of magnitude in each direction, depending on the pulse energy. The control is subsequently investigated using velocity map imaging, identifying plausible dissociation pathways leading to N + + O + . Combining the information about the N + + O + dissociation with a well-defined control objective supports the conclusion that the primary control mechanism involves selectively populating long-lived NO 2+ vibrational states.
Guidelines for creating artificial neural network empirical interatomic potential from first-principles molecular dynamics data under specific conditions and its application to $α$-Ag 2 Se
First-principles molecular dynamics (FPMD) simulations are highly accurate, but due to their high calculation cost, the computational scale is often limited to hundreds of atoms and few picoseconds under specific temperature and pressure conditions. As such, we present here the guidelines for creating artificial neural network empirical interatomic potential (ANN potential) trained with such a limited FPMD data, which can perform long time scale MD simulations at least under the same conditions. The FPMD data for training are prepared on the basis of the convergence of radial distribution function [$g(r)$]. While training the ANN using total energy and atomic forces of the FPMD data, the error of pressure is also monitored and minimized. To create further robust potential, we add a small amount of FPMD data to reproduce the interaction between two atoms that are close to each other. ANN potentials for $α$-Ag 2 Se were created as an application example, and it has been confirmed that not only $g(r)$ and mean square displacements but also the specific heat requiring a long time scale simulation matched the FPMD and the experimental values. In addition, the MD simulation using the ANN potential achieved over 10 4 acceleration over the FPMD one. The guidelines proposed here mitigate the creation difficulty of the ANN potential, and a lot of FPMD data sleeping on the hard disk after the research may be put on the front stage again.
The unusual symmetry of hexafluoro-o-xylene—A microwave spectroscopy and computational study
The rotational constants and quartic centrifugal distortion coefficients of hexafluoro-o-xylene were precisely derived from the 8 GHz to 18 GHz gas phase microwave spectrum. In addition, the rotational constants of all singly substituted 13 C isotopologues were determined. Instead of the intuitively expected symmetry of C 2v , as in o-xylene, calculations with a variety of methods (B3LYP, CAM-B3LYP, ωB97XD, MP2, and coupled-cluster singles, doubles, and perturbative triples) predict a C 2 symmetry structure in which the two CF 3 groups rotate in opposite directions by about 16°. While the experimental results in this study are not capable of proving this unusual symmetry, they can support future microwave, gas phase electron diffraction or nuclear magnetic resonance studies. From the presented data, a preliminary r 0 structure was determined, reproducing the experimental rotational constants with deviations of no more than 15 kHz. Analysis of the interactions between the two CF 3 groups using an effective fragment potential approach identifies two major contributions to their interaction, due to exchange-repulsion and electrostatic repulsion, with electrostatic repulsion responsible for the barrier at the C 2v geometry.
Watching a signaling protein function: What has been learned over four decades of time-resolved studies of photoactive yellow protein
Photoactive yellow protein (PYP) is a signaling protein whose internal p-coumaric acid chromophore undergoes reversible, light-induced trans-to-cis isomerization, which triggers a sequence of structural changes that ultimately lead to a signaling state. Since its discovery nearly 40 years ago, PYP has attracted much interest and has become one of the most extensively studied proteins found in nature. The method of time-resolved crystallography, pioneered by Keith Moffat, has successfully characterized intermediates in the PYP photocycle at near atomic resolution over 12 decades of time down to the sub-picosecond time scale, allowing one to stitch together a movie and literally watch a protein as it functions. But how close to reality is this movie? To address this question, results from numerous complementary time-resolved techniques including x-ray crystallography, x-ray scattering, and spectroscopy are discussed. Emerging from spectroscopic studies is a general consensus that three time constants are required to model the excited state relaxation, with a highly strained ground-state cis intermediate formed in less than 2.4 ps. Persistent strain drives the sequence of structural transitions that ultimately produce the signaling state. Crystal packing forces produce a restoring force that slows somewhat the rates of interconversion between the intermediates. Moreover, the solvent composition surrounding PYP can influence the number and structures of intermediates as well as the rates at which they interconvert. When chloride is present, the PYP photocycle in a crystal closely tracks that in solution, which suggests the epic movie of the PYP photocycle is indeed based in reality.
Modern quantum chemistry with [Open]Molcas
MOLCAS/OpenMolcas is an ab initio electronic structure program providing a large set of computational methods from Hartree–Fock and density functional theory to various implementations of multiconfigurational theory. This article provides a comprehensive overview of the main features of the code, specifically reviewing the use of the code in previously reported chemical applications as well as more recent applications including the calculation of magnetic properties from optimized density matrix renormalization group wave functions.
Efficient excimer-based white OLEDs with reduced efficiency roll-off
A tetradentate Pt(II) complex, Pt2O2-p2m, which exhibits both efficient monomer and excimer emission, was synthesized. Through rational device design to broaden the recombination zone, an OLED device employing Pt2O2-p2m demonstrated an impressively high peak external quantum efficiency (EQE) of 21.5% and a warm white emission with a color rendering index of 71 and Commission Internationale de L'Eclairage coordinates of (0.409, 0.458). Moreover, a reduced efficiency roll-off was also observed to retain high EQE values of 20% EQE at 1000 cd/m 2 and 17% EQE at 5000 cd/m 2 , and an LT70 (time to 70% initial luminance) was estimated to be over 150 h at 1000 cd/m2 under constant operation at accelerated driving conditions.
High-level coupled-cluster energetics by Monte Carlo sampling and moment expansions: Further details and comparisons
We recently proposed a novel approach to converging electronic energies equivalent to high-level coupled-cluster (CC) computations by combining the deterministic CC(P;Q) formalism with the stochastic configuration interaction (CI) and CC Quantum Monte Carlo (QMC) propagations. This article extends our initial study [J. E. Deustua, J. Shen, and P. Piecuch, Phys. Rev. Lett. 119, 223003 (2017)], which focused on recovering the energies obtained with the CC method with singles, doubles, and triples (CCSDT) using the information extracted from full CI QMC and CCSDT-MC, to the CIQMC approaches truncated at triples and quadruples. It also reports our first semi-stochastic CC(P;Q) calculations aimed at converging the energies that correspond to the CC method with singles, doubles, triples, and quadruples (CCSDTQ). The ability of the semi-stochastic CC(P;Q) formalism to recover the CCSDT and CCSDTQ energies, even when electronic quasi-degeneracies and triply and quadruply excited clusters become substantial, is illustrated by a few numerical examples, including the F–F bond breaking in F 2 , the automerization of cyclobutadiene, and the double dissociation of the water molecule.