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We study the influence of relative humidity (RH) on the nonlinear elastic response of granular media. Previous work has shown that the nonlinear elastic response of consolidated granular media like rocks likely arises from two distinct mechanisms; however, we do not have a clear understanding of their physical origins at the microscopic scale. Here, we conduct dynamic acousto-elastic testing (DAET) on samples of glass beads under dry (∼10%), ambient (∼60%), and humid (∼100%) conditions at room temperature and a constant static stress of 4 MPa. DAET allows us to retrieve the full nonlinear elastic response, including transient softening and hysteretic effects. We find that the elastic nonlinearity of humid samples is an order of magnitude larger than dry samples. Moreover, we find that all extracted nonlinear parameters increase with RH. This overall increase in nonlinearity is consistent with findings from previous studies and with the hypothesis that water adsorption on the grains makes the contact junctions weaker and prone to greater disturbances when subjected to dynamic stressing. Our results also suggest that, if indeed both mechanisms coexist, they are affected in a similar fashion in these glass bead samples and cannot be distinguished by varying RH. [ABSTRACT FROM AUTHOR]

Permutationally invariant polynomial (PIP) regression has been used to obtain machine-learned potential energy surfaces, including analytical gradients, for many molecules and chemical reactions. Recently, the approach has been extended to moderate size molecules with up to 15 atoms. The algorithm, including "purification of the basis," is computationally efficient for energies; however, we found that the recent extension to obtain analytical gradients, despite being a remarkable advance over previous methods, could be further improved. Here, we report developments to further compact a purified basis and, more significantly, to use the reverse differentiation approach to greatly speed up gradient evaluation. We demonstrate this for our recent four-body water interaction potential. Comparisons of training and testing precision on the MD17 database of energies and gradients (forces) for ethanol against numerous machine-learning methods, which were recently assessed by Dral and co-workers, are given. The PIP fits are as precise as those using these methods, but the PIP computation time for energy and force evaluation is shown to be 10–1000 times faster. Finally, a new PIP potential energy surface (PES) is reported for ethanol based on a more extensive dataset of energies and gradients than in the MD17 database. Diffusion Monte Carlo calculations that fail on MD17-based PESs are successful using the new PES. [ABSTRACT FROM AUTHOR]

Using the all-optical molecular orientation technique with intense nonresonant two-color laser pulses, stronger molecular orientation |⟨cos θ2D⟩| ∼ 0.34 is achieved by employing the following two strategies: (1) carbonyl sulfide molecules lying in the lower rotational states are selected using a home-built molecular deflector and (2) the rising parts of the two wavelengths of the pump pulse are adjusted by introducing a Michelson-type delay line in the optical path. The achieved degree of molecular orientation is higher than that observed in the proof-of-principle experiment [Oda et al., Phys. Rev. Lett. 104, 213901 (2010)] by about an order of magnitude and the highest ever characterized directly by Coulomb explosion imaging with appropriate probe polarization. [ABSTRACT FROM AUTHOR]

Reverse bias leakage current through 4H-SiC Schottky diodes was modeled using quantum transmission theory and the theoretically calculated values were compared with the measured values from fabricated Schottky diodes. To account for interface defects, energy barriers due to Fermi pinning from previously observed defects were used in place of the ideal barrier structure predicted by the Schottky–Mott rule. Incorporating barriers with energy values set due to Fermi pinning at known defect energies resulted in better experimental agreement by many orders of magnitude. [ABSTRACT FROM AUTHOR]

The physics of ionic electrospray propulsion spans multiple length scales. This paper combines a molecular dynamics model, a particle–particle model, and a particle-in-cell model to investigate the physics of ionic electrospray propulsion over 9 orders of magnitude in length scale. The combined models are applied to simulate beam emission for an ionic electrospray propulsion system with porous emitter tips and 1-ethyl-3-methylimidazolium tetrafluoroborate ionic liquid propellant from the emission site to the downstream plume. Additionally, the impact of multiple emission sites from a single emitter tip is analyzed with regard to extractor grid interception and overall beam neutralization for bipolar thruster pairs. Results show that beams consisting of species of different masses (i.e., monomer and dimer species) are affected by particle–particle forces during acceleration and should not be treated as a superposition of independently accelerated species in macro-scale plume models. The activation of multiple emission sites also causes a noticeable increase in the beam's spread, leading to increased intercepted current but relatively little adverse effects in the downstream plume region. [ABSTRACT FROM AUTHOR]

Coulomb interaction, following an inverse-square force-law, quantifies the amount of force between two stationary and electrically charged particles. The long-range nature of Coulomb interactions poses a major challenge to molecular dynamics simulations, which are major tools for problems at the nano-/micro-scale. Various algorithms are developed to calculate the pairwise Coulomb interactions to a linear scale, but poor scalability limits the size of simulated systems. Here, we use an efficient molecular dynamics algorithm with the random batch Ewald method on all-atom systems where the complete Fourier components in the Coulomb interaction are replaced by randomly selected mini-batches. By simulating the N-body systems up to 108 particles using 10 000 central processing unit cores, we show that this algorithm furnishes O(N) complexity, almost perfect scalability, and an order of magnitude faster computational speed when compared to the existing state-of-the-art algorithms. Further examinations of our algorithm on distinct systems, including pure water, a micro-phase separated electrolyte, and a protein solution, demonstrate that the spatiotemporal information on all time and length scales investigated and thermodynamic quantities derived from our algorithm are in perfect agreement with those obtained from the existing algorithms. Therefore, our algorithm provides a promising solution on scalability of computing the Coulomb interaction. It is particularly useful and cost-effective to simulate ultra-large systems, which is either impossible or very costly to conduct using existing algorithms, and thus will be beneficial to a broad range of problems at nano-/micro-scales. [ABSTRACT FROM AUTHOR]

Packing and crowding are used in biology as mechanisms to (self-)regulate internal molecular or cellular processes based on collective signaling. Here, we study how the transition kinetics of an internal "switch" of responsive macromolecules is modified collectively by their spatial packing. We employ Brownian dynamics simulations of a model of Responsive Colloids, in which an explicit internal degree of freedom—here, the particle size—moving in a bimodal energy landscape self-consistently responds to the density fluctuations of the crowded environment. We demonstrate that populations and transition times for the two-state switching kinetics can be tuned over one order of magnitude by "self-crowding." An exponential scaling law derived from a combination of Kramers' and liquid state perturbation theory is in very good agreement with the simulations. [ABSTRACT FROM AUTHOR]

Reducing energy consumption in the energy-intensive production systems is of great significance and attracts more and more attention. Although a lot of efforts have been devoted to formulate and solve the energy consumption optimisation problem in the Bernoulli serial lines, existing methods for solving the problem in long Bernoulli lines either cannot obtain the optimal solution or are time-consuming. For this purpose, this paper divides the problem in the long line into a set of problems in two-machine lines and proposes a computationally efficient and globally convergent algorithm to solve it. Extensive numerical experiments show that the proposed algorithm not only can optimally (in the numerical way) solve the energy consumption optimisation problem in long Bernoulli serial lines, but also is orders of magnitude more efficient than existing algorithms. [ABSTRACT FROM AUTHOR]

Multi-color terahertz (THz) detector has attracted much attention in various applications because of the ability to obtain more comprehensive information simultaneously. THz quantum well photodetectors (QWPs) have great advantages in realizing multi-color detection because of high speed, sensitivity, and mature technology. In this work, QWPs based on antenna coupled microcavity (AM-QWP) and etched antenna coupled microcavity (EAM-QWP) structures are proposed to realize multi-color THz detection. Thanks to the combination of the microcavity resonance and surface plasmon polariton mode, AM-QWP achieves a coupling efficiency of one order of magnitude higher than that of the conventional 45° edge facet coupler (45°-QWP) in multiple bands. The EAM-QWP only retains the active region where the effective photocurrent is generated so that the coupling light is highly localized in a small area, improving the optical coupling efficiency by two orders higher compared with 45°-QWP. It is theoretically estimated that the responsivity of AM-QWP and EAM-QWP at the temperature of 4 K is 9.6–24.0 A/W and 78.4–196.0 A/W while their noise equivalent power (NEP) is 5.4 × 10−4–1.1 × 10−3 pW/Hz1/2 and 1.7 × 10−5–3.5 × 10−5 pW/Hz1/2, and the specific detectivity is 4.4 × 1012–8.9 × 1012 and 6.9 × 1013–1.4 × 1014 cm Hz1/2/W, respectively. This work provides a guideline for the experimental realization of high-performance multi-color THz QWPs. [ABSTRACT FROM AUTHOR]

We present a method to perform accurate and efficient simulations of photovoltaic quantum cascade detector (QCD) structures based on the ensemble Monte Carlo (EMC) approach. Since the photocurrent is typically orders of magnitude smaller than the pump current in a quantum cascade laser (QCL), a direct application of QCL simulation techniques is not sufficiently accurate. We demonstrate that by exploiting thermodynamic equilibrium relations for the electron populations and scattering rates, the EMC method can be adapted to yield reliable results for the essential QCD figures of merit, such as responsivity and specific detectivity. The modeling approach is validated against available experimental results for various mid-infrared and terahertz QCD designs and furthermore compared to simulations based on the non-equilibrium Green's function method. [ABSTRACT FROM AUTHOR]

We introduce a tempering approach with stochastic density functional theory (sDFT), labeled t-sDFT, which reduces the statistical errors in the estimates of observable expectation values. This is achieved by rewriting the electronic density as a sum of a "warm" component complemented by "colder" correction(s). Since the warm component is larger in magnitude but faster to evaluate, we use many more stochastic orbitals for its evaluation than for the smaller-sized colder correction(s). This results in a significant reduction in the statistical fluctuations and systematic deviation compared to sDFT for the same computational effort. We demonstrate the method's performance on large hydrogen-passivated silicon nanocrystals, finding a reduction in the systematic deviation in the energy by more than an order of magnitude, while the systematic deviation in the forces is also quenched. Similarly, the statistical fluctuations are reduced by factors of ≈4–5 for the total energy and ≈1.5–2 for the forces on the atoms. Since the embedding in t-sDFT is fully stochastic, it is possible to combine t-sDFT with other variants of sDFT such as energy-window sDFT and embedded-fragmented sDFT. [ABSTRACT FROM AUTHOR]

Bose–Einstein condensate (BEC)-based atom interferometry exploits low temperatures and long coherence lengths to facilitate high-precision measurements. Progress in atom interferometry promises improvements in navigational devices like gyroscopes and accelerometers, as well as applications in fundamental physics such as accurate determination of physical constants. Previous work demonstrates that beam splitters and mirrors for coherent manipulation of dilute BEC momentum in atom interferometers can be implemented with sequences of non-resonant standing-wave light pulses. While previous work focuses on the optimization of the optical pulses' amplitude and duration to produce high-order momentum states with high fidelity, we explore how varying the shape of the optical pulses affects optimal beam-splitter performance, as well as the effect of pulse shape on the sensitivity of optimized parameters in achieving high fidelity in high-momentum states. In simulations of two-pulse beam splitters utilizing optimized square, triangle, and sinc-squared pulse shapes applied to dilute BECs, we, in some cases, reduce parameter sensitivity by an order of magnitude while maintaining fidelity. [ABSTRACT FROM AUTHOR]

Simulations of colloidal suspensions consisting of mesoscopic particles and smaller species such as ions or depletants are computationally challenging as different length and time scales are involved. Here, we introduce a machine learning (ML) approach in which the degrees of freedom of the microscopic species are integrated out and the mesoscopic particles interact with effective many-body potentials, which we fit as a function of all colloid coordinates with a set of symmetry functions. We apply this approach to a colloid–polymer mixture. Remarkably, the ML potentials can be assumed to be effectively state-independent and can be used in direct-coexistence simulations. We show that our ML method reduces the computational cost by several orders of magnitude compared to a numerical evaluation and accurately describes the phase behavior and structure, even for state points where the effective potential is largely determined by many-body contributions. [ABSTRACT FROM AUTHOR]

The multi-layer multi-configuration time-dependent Hartree (ML-MCTDH) approach can suffer from numerical instabilities whenever the wavefunction is weakly entangled. These instabilities arise from singularities in the equations of motion (EOMs) and necessitate the use of regularization of the EOMs. The Projector Splitting Integrator (PSI) has previously been presented as an approach for evolving ML-MCTDH wavefunctions that is free of singularities. Here, we will discuss the implementation of the multi-layer PSI with a particular focus on how the steps required relate to those required to implement standard ML-MCTDH. We demonstrate the efficiency and stability of the PSI for large ML-MCTDH wavefunctions containing up to hundreds of thousands of nodes by considering a series of spin-boson models with up to 106 bath modes and find that for these problems, the PSI requires roughly 3–4 orders of magnitude fewer Hamiltonian evaluations and 2–3 orders of magnitude fewer Hamiltonian applications than standard ML-MCTDH and 2–3/1–2 orders of magnitude fewer evaluations/applications than approaches that use improved regularization schemes. Finally, we consider a series of significantly more challenging multi-spin-boson models that require much larger numbers of single-particle functions with wavefunctions containing up to ∼ 1.3 × 1 0 9 parameters to obtain accurate dynamics. [ABSTRACT FROM AUTHOR]

The evaluation of nucleation rates from molecular dynamics trajectories is hampered by the slow nucleation time scale and impact of finite size effects. Here, we show that accurate nucleation rates can be obtained in a very general fashion relying only on the free energy barrier, transition state theory, and a simple dynamical correction for diffusive recrossing. In this setup, the time scale problem is overcome by using enhanced sampling methods, in casu metadynamics, whereas the impact of finite size effects can be naturally circumvented by reconstructing the free energy surface from an appropriate ensemble. Approximations from classical nucleation theory are avoided. We demonstrate the accuracy of the approach by calculating macroscopic rates of droplet nucleation from argon vapor, spanning 16 orders of magnitude and in excellent agreement with literature results, all from simulations of very small (512 atom) systems. [ABSTRACT FROM AUTHOR]

The coupled cluster iteration scheme is analyzed as a multivariate discrete time map using nonlinear dynamics and synergetics. The nonlinearly coupled set of equations to determine the cluster amplitudes are driven by a fraction of the entire set of cluster amplitudes. These driver amplitudes enslave all other amplitudes through a synergistic inter-relationship, where the latter class of amplitudes behave as the auxiliary variables. The driver and the auxiliary variables exhibit vastly different time scales of relaxation during the iteration process to reach the fixed points. The fast varying auxiliary amplitudes are small in magnitude, while the driver amplitudes are large, and they have a much longer time scale of relaxation. Exploiting their difference in relaxation time scale, we employ an adiabatic decoupling approximation, where each of the fast relaxing auxiliary modes is expressed as a unique function of the principal amplitudes. This results in a tremendous reduction in the independent degrees of freedom. On the other hand, only the driver amplitudes are determined accurately via exact coupled cluster equations. We will demonstrate that the iteration scheme has an order of magnitude reduction in computational scaling than the conventional scheme. With a few pilot numerical examples, we would demonstrate that this scheme can achieve very high accuracy with significant savings in computational time. [ABSTRACT FROM AUTHOR]

Numerous investigations on plasma–liquid interaction have been published in the literature using various reactor geometries. However, our understanding of the basic configuration of a pin-to-plane dielectric barrier discharge (DBD) in contact with water is still incomplete. We, therefore, performed the electrical diagnostics of such a discharge, operated in an AC regime with sinusoidal high voltage, focusing mainly on the power injected into the plasma in relation with several experimental parameters. It was found that the injected power increased linearly with the amplitude of the applied voltage, while without water, the evolution followed a second-order polynomial. In both cases, the discharge power was proportional approximately with the frequency. For the DBD above water, the power was about three times greater than that without water for the same air gap. It was observed that changing the discharge gap from 1 to 5 mm led to a slight increase in power by only 15%. The water conductivity also influenced the power injected into the plasma only to a small extent. Thus, the variation in water conductivity over four orders of magnitude determined a fluctuation in discharge power of ±20%. [ABSTRACT FROM AUTHOR]

Classical molecular dynamics (MD) and imaginary-time path-integral dynamics methods underestimate the infrared absorption intensities of overtone and combination bands by typically an order of magnitude. Plé et al. [J. Chem. Phys. 155, 2863 (2021)] have shown that this is because such methods fail to describe the coupling of the centroid to the Matsubara dynamics of the fluctuation modes; classical first-order perturbation theory (PT) applied to the Matsubara dynamics is sufficient to recover most of the lost intensity in simple models and gives identical results to quantum (Rayleigh–Schrödinger) PT. Here, we show numerically that the results of this analysis can be used as post-processing correction factors, which can be applied to realistic (classical MD or path-integral dynamics) simulations of infrared spectra. We find that the correction factors recover most of the lost intensity in the overtone and combination bands of gas-phase water and ammonia and much of it for liquid water. We then re-derive and confirm the earlier PT analysis by applying canonical PT to Matsubara dynamics, which has the advantage of avoiding secular terms and gives a simple picture of the perturbed Matsubara dynamics in terms of action-angle variables. Collectively, these variables "Matsubara heat" the amplitudes of the overtone and combination vibrations of the centroid to what they would be in a classical system with the oscillators (of frequency Ωi) held at their quantum effective temperatures [of ℏΩi coth(βℏΩi/2)/2kB]. Numerical calculations show that a similar neglect of "Matsubara heating" causes path-integral methods to underestimate Fermi resonance splittings. [ABSTRACT FROM AUTHOR]

We report a generally applicable computational and experimental approach to determine vibronic branching ratios in linear polyatomic molecules to the 10−5 level, including for nominally symmetry-forbidden transitions. These methods are demonstrated in CaOH and YbOH, showing approximately two orders of magnitude improved sensitivity compared with the previous state of the art. Knowledge of branching ratios at this level is needed for the successful deep laser cooling of a broad range of molecular species. [ABSTRACT FROM AUTHOR]

In the recent past, high-refractive index nano- and micropillars have been widely used for significantly enhancing the fluorescence properties of quantum emitters embedded within the pillar. However, a complete study of the electromagnetic dynamics and nanophotonics of single-photon emission inside the high-refractive index nanopillars is currently missing. In order to design nano- and micropillars for the fluorescence enhancement of embedded quantum emitters, it is essential to understand their emission dynamics once single-photon emitters are embedded inside them. Here, both analytically and computationally, we study the electromagnetic dynamics of the nitrogen-vacancy (NCVSi) centers in silicon-carbide (SiC) micro-pillars due to their characteristic emission in the optical O-band telecommunication region (1260–1360 nm). For efficient micro-pillar design, the fluorescence enhancement was determined to increase by more than two orders of magnitude with the collection efficiency reaching about 40% from a very low value of ∼0.5% in bulk SiC. Presently, the enhancement achieved experimentally is limited to a factor of around 10–20. Our results are, therefore, expected to accelerate research in the field quantum emitters coupling to micro-pillars or micro-pillar photonics. [ABSTRACT FROM AUTHOR]

A new integration scheme for ab initio molecular dynamics (MD) is proposed in this work for efficient propagation using large time steps (e.g., 2.0 fs or a larger time step with one ab initio evaluation of gradients for the dynamics point and one additional evaluation for the anchor point per dynamics step). This algorithm is called re-integration with anchor points (REAP) integrator. The REAP integrator starts from a quadratic potential energy surface based on the updated Hessian to propagate the system to the halfway of the MD step that is called the anchor point. Then, an approximate dynamics position for this step is obtained by the propagation based on an interpolated surface using the anchor point and the previous MD point. The approximate dynamics step can be further improved by the re-integration steps, i.e., integration based on the interpolated surface using the calculated energies, gradients, and updated Hessians of the previous step, the anchor point, and the approximate current step. A trajectory only needs one analytical Hessian calculation at the initial geometry, and thereafter, only calculations of gradients are required. This integrator can be considered either as a generalization of Hessian-based predictor–corrector integration with substantial improvement of accuracy and efficiency or as a dynamics on interpolated surfaces that are built on the fly. An automatic correction scheme is implemented by comparing the interpolated energies and gradients to the actual ones to ensure the quality of the interpolations at a certain level. The tests in this work show that the REAP method can increase computational efficiency by more than one order of magnitude than that of the velocity Verlet integrator and more than twice that of Hessian-based predictor–corrector integration. [ABSTRACT FROM AUTHOR]

In situ transport measurements on 5.8–92.1 nm thick epitaxial Ti4SiC3(0001) layers are used to experimentally verify the previously predicted low resistivity scaling. Magnetron co-sputtering from three elemental sources at 1000 °C onto 12-nm-thick TiC(111) nucleation layers on Al2O3(0001) substrates yields epitaxial growth with Ti4SiC3(0001) || Al2O3(0001) and Ti4SiC3(10 1 ¯ 0) || Al2O3(2 1 ¯ 1 ¯ 0), a low and thickness-independent surface roughness of 0.6 ± 0.2 nm, and a measured stoichiometric composition. The room-temperature resistivity ρ increases slightly with decreasing thickness, from ρ = 35.2 ± 0.4 to 37.5 ± 1.1 μΩ cm for d = 92.1–5.8 nm, and similarly from 9.5 ± 0.2 to 11.0 ± 0.4 μΩ cm at 77 K, indicating only a minor effect of electron surface scattering on ρ. Data analysis with the classical Fuchs–Sondheimer model yields a room-temperature bulk resistivity ρo = 35.1 ± 0.4 μΩ cm in the basal plane and suggests effective mean free paths λ = 1.1 ± 0.6 at 293 K and λ = 3.0 ± 2.0 nm at 77 K if assuming completely diffuse electron surface scattering. First-principles calculations predict an anisotropic Ti4SiC3 Fermi surface and a product ρoλ = 19.3 × 10−16 Ω m2 in the basal plane. This value is six times larger than that predicted previously and five times larger than the measured temperature-independent effective ρoλ = (3.8 ± 2.1) × 10−16 Ω m2. This deviation can be explained by a high experimental electron scattering specularity of p = 0.8 for Ti4SiC3(0001) surfaces. Air exposure causes a 4% room-temperature resistivity increase for d = 5.8 nm, indicating a decrease in the surface scattering specularity Δp = −0.19. The overall results show that Ti4SiC3 is not directly applicable as an interconnect material due to its relatively large ρo. However, the particularly small resistivity scaling with an effective λ that is more than an order of magnitude smaller than that of Cu confirms the potential of MAX phase materials for high-conductivity narrow interconnects. [ABSTRACT FROM AUTHOR]

The space charge effect is important in free-electron devices and sometimes plays a key role. A vacuum-compatible micromanipulation platform was devised to study this effect in a diode structure while changing the width of the gap between the emitter and the collector in situ in the range of hundreds of micrometers to tens of micrometers. The current–voltage characteristics were found to upshift with a decrease in the interelectrode distance; the space charge-limited current increased by approximately two orders of magnitude when the interelectrode distance decreased from 550 to 50 μm. The simplicity of the parallel-plate structure enabled analysis based on one-dimensional emission and transport with the measurement results showing a good fit to the model by Longo combined with the Child–Langmuir theory. [ABSTRACT FROM AUTHOR]

In this study, the formation and character of gallium vacancies (VGa) and their complexes in near surface and bulk regions of single crystal β-Ga2O3 were explored using unintentionally doped single crystals grown by the Czochralski method. As-grown and O2 annealed (up to 1550 °C) samples were investigated using positron annihilation spectroscopy (PAS) to study the top 0.05–6 μm, and also current–voltage measurements and infrared (IR) spectroscopy, with hydrogenated samples to probe VGa, to study the bulk. After annealing in O2 > 1000 °C, the β-Ga2O3 resistivity begins increasing, up to ∼109 Ω cm for 1550 °C treatment, with the top 0.5 mm being many orders of magnitude more resistive. PAS measurements of the top 6 μm (S values) and very near surface 200 nm (diffusion length, L) indicate differential behavior as a function of peak annealing temperature. At least four temperature regimes of behavior are described. VGa are present in the bulk after growth, but considerable changes occur upon annealing at a temperature ≈1000 °C, where L and S decrease simultaneously, suggesting an increasing defect concentration (L) but a decreasing defect volume (S). Annealing at a temperature ≈1400 °C increases S again, showing an increasing volume concentration of VGa, with IR absorption showing a large signature of VGa-2H, indicative of increased VGa formation that was not present when annealing at a temperature ≈1000 °C. These results suggest that defect changes from annealing in oxygen are depth dependent, and that VGa configuration may not be the same near the oxygen-exposed surface of the sample and in the bulk. [ABSTRACT FROM AUTHOR]

Hydrogenation of tungsten trioxide (WO3) can effectively modulate its material property and induce the insulator–metal transition. Due to the insertion of H atoms, a transparent WO3 film will normally change to deep-blue color because of its pronounced electrochromism. More importantly, the electronic structure will also convert from an insulator to a metallic state, showing greatly improved conductivity with an enhancement of up to six orders of magnitude. Combined with the traditional lithography route, selective hydrogenation of WO3 in microscale size is achieved based on the electron–proton synergistic effect in an acid solution. This metal-like conductive H-doped WO3 can be used as an erasable microcircuit since it will be recovered to a WO3 insulator by annealing in air at an appropriate temperature. The current study demonstrates a facile way to fabricate erasable WO3 conducting micro/nanowires, or even microcircuits, by selective hydrogenation under ambient conditions, which should be extended to other oxide materials for functional applications. [ABSTRACT FROM AUTHOR]

We utilize atomistic simulations that account for point charges and dipoles to demonstrate that flexoelectricity, which arises from strain gradients, can be exploited to generate electricity from crumpled graphene sheets. Indentation of a circular graphene sheet generates localized developable (d)-cones, for which we verify the core radius and azimuthal angle with established theoretical models. We determine the voltage that can be generated based on the resulting electrostatic fields and compare the voltage generation to previous theoretical predictions that are scaled down to the nanoscale. In doing so, we find that the voltage generated from crumpling graphene exceeds, by about an order of magnitude, the expected voltage generation, indicating the benefit of exploiting the large strain gradients that are possible at the nanoscale. Finally, we demonstrate that crumpling may be a superior mechanism of flexoelectric energy generation as compared to bending of two-dimensional nanomaterials. [ABSTRACT FROM AUTHOR]

The YbOH triatomic molecule can be efficiently used to measure the electron electric dipole moment, which violates time-reversal (T) and spatial parity (P) symmetries of fundamental interactions [Kozyryev and Hutzler, Phys. Rev. Lett. 119, 133002 (2017)]. We study another mechanism of the T, P-violation in the YbOH molecule—the electron–electron interaction mediated by the low-mass axionlike particle. For this, we calculate the molecular constant that characterizes this interaction and use it to estimate the expected magnitude of the effect to be measured. It is shown that this molecular constant has the same order of magnitude as the corresponding molecular constant corresponding to the axion-mediated electron–nucleus interaction. According to our estimation, an experiment on YbOH will allow one to set updated laboratory constraints on the CP-violating electron–axion coupling constants. [ABSTRACT FROM AUTHOR]

The lattice thermal conductivity of carbon materials is particularly interesting because it can vary within a range spanning five orders of magnitude depending on the atomic configuration. Herein, we systematically study the lattice thermal conductivity and phonon transport properties of pentadiamond, a new three-dimensional carbon allotrope consisting of pentagonal carbon rings. Based on first-principles calculations and an iterative solution to the linearized Boltzmann transport equation, the intrinsic lattice thermal conductivity (kl) is found to be 490.88 W/mK at room temperature, much lower than 2664.93 W/mK of diamond. A detailed analysis of both harmonic and anharmonic properties reveals that the low kl of pentadiamond essentially originates from its large phonon phase space, short phonon relaxation time resulting from strong overlap between the acoustic and low-lying optical phonon branches, and the low phonon group velocity. The distinct thermal transport behavior exhibited in pentadiamond further shows the diversity and complexity in lattice thermal conductivity of carbon allotropes. [ABSTRACT FROM AUTHOR]

The crystallization of sputter-deposited substrate-free films of amorphous germanium was induced by electron irradiation at SEM-level energies of less than 20 keV at ambient temperature using an electron probe microanalyzer. Instantaneous crystallization, referred to as explosive crystallization, occurred consistently at 2–20 keV; the threshold of electron fluxes is 1015–1016 m−2 s−1, which is five to six orders of magnitude lower than those at 100 keV reported previously. This process is expected to be advantageous in the production of polycrystalline Ge films since it is rapid, requires little energy, and results in negligible damage to the substrate. [ABSTRACT FROM AUTHOR]

We report on the modulation characteristics of the uncooled terahertz (THz) and infrared (IR) detectors using uniform graphene layers (GLs) and perforated graphene layers (PGL). Our analysis shows that the PGL detectors could have more than an order of magnitude smaller dark current compared to more conventional GL reversed biased photodetectors operating in the same frequency range. The modulation mechanism for the simulated photodetectors is the variation of the density and effective temperature of the two-dimensional electron–hole plasma with the varying intensity of the THz or IR radiation. Our simulations predict a reasonable modulation depth up to the modulation frequencies of 50 GHz for the impinging radiation frequencies up to the mid-IR range. [ABSTRACT FROM AUTHOR]

The surface of ice in contact with water contains sites that undergo deprotonation and protonation and can act as adsorption sites for aqueous ions. Therefore, an electrical double layer should form at this interface and existing models for describing the electrical double layer at metal oxide–water interfaces should be able to be modified to describe the surface charge, surface potential, and ionic occupancy at the ice–water interface. I used a surface complexation model along with literature measurements of the zeta potential of ice in brines of various strength and pH to constrain equilibrium constants. I then made predictions of ion site occupancy, surface charge density, and partitioning of counterions between the Stern and diffuse layers. The equilibrium constant for cation adsorption is more than 5 orders of magnitude larger than the other constants, indicating that this reaction dominates even at low salinity. Deprotonated OH sites are predicted to be slightly more abundant than dangling O sites, consistent with previous work. Surface charge densities are on the order of ±0.001 C/m2 and are always negative at the moderate pH values of interest to atmospheric and geophysical applications (6–9). In this pH range, over 99% of the counterions are contained in the Stern layer. This suggests that diffuse layer polarization will not occur because the ionic concentrations in the diffuse layer are nearly identical to those in the bulk electrolyte and that electrical conduction and polarization in the Stern layer will be negligible due to reduced ion mobility. [ABSTRACT FROM AUTHOR]

Understanding water transport mechanisms at the nanoscale level remains a challenge for theoretical chemical physics. Major advances in chemical synthesis have allowed us to discover new artificial water channels, rivaling with or even surpassing water conductance and selectivity of natural protein channels. In order to interpret experimental features and understand microscopic determinants for performance improvements, numerical approaches based on all-atom molecular dynamics simulations and enhanced sampling methods have been proposed. In this study, we quantify the influence of microscopic observables, such as channel radius and hydrogen bond connectivity, and of meso-scale features, such as the size of self-assembly blocks, on the permeation rate of a self-assembled nanocrystal-like artificial water channel. Although the absolute permeation rate extrapolated from these simulations is overestimated by one order of magnitude compared to the experimental measurement, the detailed analysis of several observed conductive patterns in large assemblies opens new pathways to scalable membranes with enhanced water conductance for the future design. [ABSTRACT FROM AUTHOR]

The recently discovered large flexoelectricity in relaxor ferroelectrics has rekindled considerable research interest. In this paper, several Sm-doped Pb(Mg2/3Nb1/3)O3–xPbTiO3 (PMN–xPT) ferroelectric ceramics were prepared and the relationship between flexoelectricity and PT content was systematically investigated. The largest flexoelectric response (∼550 μC/m) was observed in the Sm-doped PMN–32PT ceramic, which should be accounted for in the reorientation of the polar nanoregions. At room temperature, the flexoelectric response of Sm-doped PMN–32PT ceramic is an order of magnitude higher than that of the parent PMN–PT ceramics and even 50% higher than that of Bi–PMN–32PT ceramic (∼300 μC/m). Such a big increment is directly related to the greater local structural heterogeneity caused by Sm3+ ions into PMN–PT. Therefore, the result presented in this paper verifies that introducing local structural heterogeneity is a feasible approach to achieve ultrahigh flexoelectricity. [ABSTRACT FROM AUTHOR]

Single-ion Soret coefficients αi characterize the tendency of ions in an electrolyte solution to move in a thermal gradient. When these coefficients differ between cations and anions, an electric field can be generated. For this so-called electrolyte Seebeck effect to occur, different thermodiffusive fluxes need to be blocked by boundaries—electrodes, for example. Local charge neutrality is then broken in the Debye-length vicinity of the electrodes. Confusingly, many authors point to these regions as the source of the thermoelectric field yet ignore them in derivations of the time-dependent Seebeck coefficient S(t), giving a false impression that the electrolyte Seebeck effect is purely a bulk phenomenon. Without enforcing local electroneutrality, we derive S(t) generated by a binary electrolyte with arbitrary ionic valencies subject to a time-dependent thermal gradient. Next, we experimentally measure S(t) for five acids, bases, and salts near titanium electrodes. For the steady state, we find S ≈ 2 mV K−1 for many electrolytes, roughly one order of magnitude larger than the predictions based on literature αi. We fit our expression for S(t) to the experimental data, treating the αi as fit parameters, and also find larger-than-literature values, accordingly. [ABSTRACT FROM AUTHOR]

The amount of cross-linking in the design of polymer materials is a key parameter for the modification of numerous physical properties, importantly, the permeability to molecular solutes. We consider networks with a diamond-like architecture and different cross-link ratios, concurring with a wide range of the polymer volume fraction. We particularly focus on the effect and the competition of two independent component-specific solute–polymer interactions, i.e., we distinguish between chain-monomers and cross-linkers, which individually act on the solutes and are altered to cover attractive and repulsive regimes. For this purpose, we employ coarse-grained, Langevin computer simulations to study how the cross-link ratio of polymer networks controls the solute partitioning, diffusion, and permeability. We observe different qualitative behaviors as a function of the cross-link ratio and interaction strengths. The permeability can be tuned ranging over two orders of magnitude relative to the reference bulk permeability. Finally, we provide scaling theories for the partitioning and diffusion that explicitly account for the component-specific interactions as well as the cross-link ratio and the polymer volume fraction. These are in overall good agreement with the simulation results and grant insight into the underlying physics, rationalizing how the cross-link ratio can be exploited to tune the solute permeability of polymeric networks. [ABSTRACT FROM AUTHOR]

Though additive manufacturing and novel optimization techniques have led to many recent advances in elastic metamaterials, difficult fundamental challenges (e.g., narrow bandgaps) and practical challenges (e.g., dissipation and friction) remain. This work introduces simple and hierarchical resonant metamaterials made of soft polydimethylsiloxane rubber and removable steel insets. The additively manufactured samples are able to produce bandgaps with a gap–midgap ratio of 81.8%, which surpasses the majority of resonant, metamaterials of the same class and greatly outperforms analogous resonant structures with a stiff epoxy matrix. The role of several physical features on the transmission loss (TL) curve is assessed in detail numerically and compared to the experimental TL data. Matrix compliance is found to be a rich mechanism for bandgap widening with a dual effect: it deepens the traditional resonant bandgaps, and it can selectively shift certain vibrational modes to lower frequencies and aid in the merging of multiple bandgaps. This can lead to an overall increase of the bandgap width of over an order of magnitude. Viscous dissipation, friction, and the stochastic nature of geometrical inaccuracies common in additive manufacturing were also found to shape the TL curve and associated bandgaps to various degrees. Some of these mechanisms, combined with a soft frame, can further help merge bandgaps in rainbow or hierarchical designs and form ultrabroad, subwavelength bandgaps. [ABSTRACT FROM AUTHOR]

Variational quantum Monte Carlo (QMC) is an ab initio method for solving the electronic Schrödinger equation that is exact in principle, but limited by the flexibility of the available Ansätze in practice. The recently introduced deep QMC approach, specifically two deep-neural-network Ansätze PauliNet and FermiNet, allows variational QMC to reach the accuracy of diffusion QMC, but little is understood about the convergence behavior of such Ansätze. Here, we analyze how deep variational QMC approaches the fixed-node limit with increasing network size. First, we demonstrate that a deep neural network can overcome the limitations of a small basis set and reach the mean-field (MF) complete-basis-set limit. Moving to electron correlation, we then perform an extensive hyperparameter scan of a deep Jastrow factor for LiH and H4 and find that variational energies at the fixed-node limit can be obtained with a sufficiently large network. Finally, we benchmark MF and many-body Ansätze on H2O, increasing the fraction of recovered fixed-node correlation energy of single-determinant Slater–Jastrow-type Ansätze by half an order of magnitude compared to previous variational QMC results, and demonstrate that a single-determinant Slater–Jastrow-backflow version of the Ansatz overcomes the fixed-node limitations. This analysis helps understand the superb accuracy of deep variational Ansätze in comparison to the traditional trial wavefunctions at the respective level of theory and will guide future improvements of the neural-network architectures in deep QMC. [ABSTRACT FROM AUTHOR]

Time-resolved studies have so far relied on rapidly triggering a photo-induced dynamic in chemical or biological ions or molecules and subsequently probing them with a beam of fast moving photons or electrons that crosses the studied samples in a short period of time. Hence, the time resolution of the signal is mainly set by the pulse duration of the pump and probe pulses. In this paper, we propose a different approach to this problem that has the potential to consistently achieve orders of magnitude higher time resolutions than what is possible with laser technology or electron beam compression methods. Our proposed approach relies on accelerating the sample to a high speed to achieve relativistic time dilation. Probing the time-dilated sample would open up previously inaccessible time resolution domains. [ABSTRACT FROM AUTHOR]

We report ionic current and double-stranded DNA (dsDNA) translocation measurements through solid-state membranes with two TEM-drilled ∼3-nm diameter silicon nitride nanopores in parallel. Nanopores are fabricated with similar diameters but varying in effective thicknesses (from 2.6 to 10 nm) ranging from a thickness ratio of 1:1 to 1:3.75, producing distinct conductance levels. This was made possible by locally thinning the silicon nitride membrane to shape the desired topography with nanoscale precision using electron beam lithography (EBL). Two nanopores are engineered and subsequently drilled in either the EBL-thinned or the surrounding membrane region. By designing the interpore separation a few orders of magnitude larger than the pore diameter (e.g., ∼900 vs 3 nm), we show analytically, numerically, and experimentally that the total conductance of the two pores is the sum of the individual pore conductances. For a two-pore device with similar diameters yet thicknesses in the ratio of 1:3, a ratio of ∼1:2.2 in open-pore conductances and translocation current signals is expected, as if they were measured independently. Introducing dsDNA as analytes to both pores simultaneously, we detect more than 12 000 events within 2 min and trace them back with a high likelihood to which pore the dsDNA translocated through. Moreover, we monitor translocations through one active pore only when the other pore is clogged. This work demonstrates how two-pore devices can fundamentally open up a parallel translocation reading system for solid-state nanopores. This approach could be creatively generalized to more pores with desired parameters given a sufficient signal-to-noise ratio. [ABSTRACT FROM AUTHOR]

We find an l = 2 shape resonance fingerprinted in the angular distribution of the cold (∼1 K) Δj = 2 rotationally inelastic collision of D2 with He in a single supersonic expansion. The Stark-induced adiabatic Raman passage is used to prepare D2 in the (v = 2, j = 2) rovibrational level with control of the spatial distribution of the bond axis of the molecule by magnetic sublevel selection. We show that the rate of Δj = 2 D2–D2 relaxation is nearly two orders of magnitude weaker than that of D2–He. This suggests that the strong D2–He scattering is caused by an orbiting resonance that is highly sensitive to the shape of the long-range potential. [ABSTRACT FROM AUTHOR]

Multi-configurational time-dependent Hartree (MCTDH) calculations using time-dependent grid representations can be used to accurately simulate high-dimensional quantum dynamics on general ab initio potential energy surfaces. Employing the correlation discrete variable representation, sets of direct product type grids are employed in the calculation of the required potential energy matrix elements. This direct product structure can be a problem if the coordinate system includes polar and azimuthal angles that result in singularities in the kinetic energy operator. In the present work, a new direct product-type discrete variable representation (DVR) for arbitrary sets of polar and azimuthal angles is introduced. It employs an extended coordinate space where the range of the polar angles is taken to be [−π, π]. The resulting extended space DVR resolves problems caused by the singularities in the kinetic energy operator without generating a very large spectral width. MCTDH calculations studying the F·CH4 complex are used to investigate important properties of the new scheme. The scheme is found to allow for more efficient integration of the equations of motion compared to the previously employed cot-DVR approach [G. Schiffel and U. Manthe, Chem. Phys. 374, 118 (2010)] and decreases the required central processing unit times by about an order of magnitude. [ABSTRACT FROM AUTHOR]

The onset of shear thinning and the transition from Newtonian to non-Newtonian behavior in the viscous flow of select chalcogenide and oxide network glass-forming liquids in the deeply supercooled regime and its temperature dependence are studied using parallel plate rheometry. In all cases, the onset occurs at a shear rate γ ̇ c that is several orders of magnitude lower than the shear relaxation rate τ 0 − 1 and the former increases with increasing temperature. These results are in good qualitative agreement with the predictions of the existing models of shear relaxation and shear thinning based on the nonlinear Langevin equation theory, random first order transition theory, and the free volume model. However, in contrast to the theoretical predictions, the reduced shear rate W0 (= τ 0 γ ̇ c ) at the onset is found to range between 10−3 and 10−5 and decrease with increasing temperature. This temperature dependence becomes stronger with increasing fragility of the liquid. These results likely indicate that the shear thinning mechanism in network liquids could be fundamentally different from those in molecular, metallic, or polymeric glass-formers. [ABSTRACT FROM AUTHOR]

Ionizing radiation has the potential to cause operational disruptions and destroy microelectronic devices. This paper introduces and demonstrates a method of hardening microelectronic devices for sustained use in applications where exposure to ionizing radiation exists. By incorporating quantum structures below active regions of devices, gettering of charges created by ionizing radiation becomes possible. The gettering of electrons and holes forces recombination of carriers, thus eliminating photocurrent surges and trap filling which would otherwise disrupt device operation. Experimental results discussed here show a reduction in photocurrent of over two orders of magnitude when utilizing energy band engineering to create quantum structures for charge gettering. In this work, a nitride-based high electron mobility two-dimensional electron gas demonstrates the method. However, the theory utilized pertains not only to nitride-based devices, but transfers to other materials as well. [ABSTRACT FROM AUTHOR]

A single crystal of Fe (0.3%)-doped BaTiO3 was grown by a top-seeded solution growth method, and the photovoltaic (PV) properties (at 3.1 eV) in a multi-domain state with a 90° domain structure are investigated. We show that the overall behavior can be well understood by an analytical expression of the domain wall (DW)-PV effect superimposed on the bulk-PV effect. The fitting of photocurrents as a function of light polarization reveals that the offset component of the DW-PV effect is much larger than that of the bulk-PV effect, even though the volume fraction of the DW region is extremely small. A local electric field in the DW region is estimated to be several hundred kV cm−1, which is three orders of magnitude higher than the effective field inside the domains. [ABSTRACT FROM AUTHOR]

We report on a theoretical study of second-harmonic generation (SHG) in plasmonic nanostructures interacting with two-level quantum emitters (QEs) under incoherent energy pump. We generalize the driven-dissipative Tavis–Cummings model by introducing the anharmonic surface plasmon-polariton (SPP) mode coupled to QEs and examine physical properties of corresponding SPP-QE polariton states. Our calculations of the SHG efficiency for strong QE-SPP coupling demonstrate orders of magnitude enhancement facilitated by the polariton gain. We further discuss time-domain numerical simulations of SHG in a square lattice comprising Ag nanopillars coupled to QEs utilizing a fully vectorial nonperturbative nonlinear hydrodynamic model for conduction electrons coupled to Maxwell–Bloch equations for QEs. The simulations support the idea of gain enhanced SHG and show orders of magnitude increase in the SHG efficiency as the QEs are tuned in resonance with the lattice plasmon mode and brought above the population inversion threshold by incoherent pumping. By varying pump frequency and tuning QEs to a localized plasmon mode, we demonstrate further enhancement of the SHG efficiency facilitated by strong local electric fields. The incident light polarization dependence of the SHG is examined and related to the symmetries of participating plasmon modes. [ABSTRACT FROM AUTHOR]

This work presents algorithms for the efficient enumeration of configuration spaces following Boltzmann-like statistics, with example applications to the calculation of non-radiative rates, and an open-source implementation. Configuration spaces are found in several areas of physics, particularly wherever there are energy levels that possess variable occupations. In bosonic systems, where there are no upper limits on the occupation of each level, enumeration of all possible configurations is an exceptionally hard problem. We look at the case where the levels need to be filled to satisfy an energy criterion, for example, a target excitation energy, which is a type of knapsack problem as found in combinatorics. We present analyses of the density of configuration spaces in arbitrary dimensions and how particular forms of kernel can be used to envelope the important regions. In this way, we arrive at three new algorithms for enumeration of such spaces that are several orders of magnitude more efficient than the naive brute force approach. Finally, we show how these can be applied to the particular case of internal conversion rates in a selection of molecules and discuss how a stochastic approach can, in principle, reduce the computational complexity to polynomial time. [ABSTRACT FROM AUTHOR]

Photonic devices stand to benefit from the development of chromophores with tunable, precisely controlled spontaneous emission lifetimes. Here, we demonstrate a method to continuously tune the radiative emission lifetimes of a class of chromophores by varying the density of electronic states involved in the emission process. In particular, we examined the peculiar composition-dependent electronic structure of copper doped CdZnSe quantum dots. It is shown that the nature and density of electronic states involved with the emission process is a function of copper inclusion level, providing a very direct handle for controlling the spontaneous lifetimes. The spontaneous emission lifetimes are estimated by examining the ratios of emission lifetimes to absolute quantum yields and also measured directly by ultrafast luminescence upconversion experiments. We find excellent agreement between these classes of experiments. This scheme enables us to tune spontaneous emission lifetimes by three orders of magnitude from ∼15 ns to over ∼7 µs, which is unprecedented in existing lumophores. [ABSTRACT FROM AUTHOR]

The recently proposed r2SCAN meta-generalized-gradient approximation (mGGA) of Furness and co-workers is used to construct an efficient composite electronic-structure method termed r2SCAN-3c. To this end, the unaltered r2SCAN functional is combined with a tailor-made triple-ζ Gaussian atomic orbital basis set as well as with refitted D4 and geometrical counter-poise corrections for London-dispersion and basis set superposition error. The performance of the new method is evaluated for the GMTKN55 database covering large parts of chemical space with about 1500 data points, as well as additional benchmarks for non-covalent interactions, organometallic reactions, and lattice energies of organic molecules and ices, as well as for the adsorption on polar salt and non-polar coinage-metal surfaces. These comprehensive tests reveal a spectacular performance and robustness of r2SCAN-3c: It by far surpasses its predecessor B97-3c at only twice the cost and provides one of the best results of all semi-local density-functional theory (DFT)/QZ methods ever tested for the GMTKN55 database at one-tenth of the cost. Specifically, for reaction and conformational energies as well as non-covalent interactions, it outperforms prominent hybrid-DFT/QZ approaches at two to three orders of magnitude lower cost. Perhaps, the most relevant remaining issue of r2SCAN-3c is self-interaction error (SIE), owing to its mGGA nature. However, SIE is slightly reduced compared to other (m)GGAs, as is demonstrated in two examples. After all, this remarkably efficient and robust method is chosen as our new group default, replacing previous composite DFT and partially even expensive high-level methods in most standard applications for systems with up to several hundreds of atoms. [ABSTRACT FROM AUTHOR]

A previously published neural network potential for the description of protonated water clusters up to the protonated water tetramer, H+(H2O)4, at an essentially converged coupled cluster accuracy [C. Schran, J. Behler, and D. Marx, J. Chem. Theory Comput. 16, 88 (2020)] is applied to the protonated water hexamer, H+(H2O)6—a system that the neural network has never seen before. Although being in the extrapolation regime, it is shown that the potential not only allows for quantum simulations from ultra-low temperatures ∼1 K up to 300 K but is also able to describe the new system very accurately compared to explicit coupled cluster calculations. This transferability of the model is rationalized by the similarity of the atomic environments encountered for the larger cluster compared to the environments in the training set of the model. Compared to the interpolation regime, the quality of the model is reduced by roughly one order of magnitude, but most of the difference to the coupled cluster reference comes from global shifts of the potential energy surface, while local energy fluctuations are well recovered. These results suggest that the application of neural network potentials in extrapolation regimes can provide useful results and might be more general than usually thought. [ABSTRACT FROM AUTHOR]

Carbon nanotubes (CNTs) are the emerging alternative for silicon for developing miniatured electromechanical devices in the More than Moore's era. But, the inconsistent pitch distances among the aligned CNTs have limited their outstanding performances. Except for the intertube overlapping, the curved morphology is an important but often ignored factor for the attractive CNTs under van der Waals interaction. Here, we have synthesized a clean and curved CNT structure with a definite curvature radius by introducing micro perturbation. Electrical measurement has demonstrated that the curved structure will limit the on/off ratio by orders of magnitude but can maintain a high output delivery in transistors. This is attributed to the resistance induced by the localized strain and the extra current delivery capability of the inner walls, which can be well explained by the energy band diagram model. Among the curved CNTs, incommensurate double walled CNTs of higher diameter difference are the optimal candidates for delivering a high current output by limiting intertube charge transfer. Our demonstrations and analysis have highlighted the importance of controlling both the chiral structures and morphology of CNTs for the applications of high-performance carbon-based electronics. [ABSTRACT FROM AUTHOR]