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At least 1,459 records · Page 81

Ultrathin ferroic HfO 2 –ZrO 2 superlattice gate stack for advanced transistors

With the scaling of lateral dimensions in advanced transistors, an increased gate capacitance is desirable both to retain the control of the gate electrode over the channel and to reduce the operating voltage. This led to a fundamental change in the gate stack in 2008, the incorporation of high-dielectric-constant HfO 2 , which remains the material of choice to date. Here we report HfO 2 –ZrO 2 superlattice heterostructures as a gate stack, stabilized with mixed ferroelectric–antiferroelectric order, directly integrated onto Si transistors, and scaled down to approximately 20 ångströms, the same gate oxide thickness required for high-performance transistors. The overall equivalent oxide thickness in metal–oxide–semiconductor capacitors is equivalent to an effective SiO 2 thickness of approximately 6.5 ångströms. Such a low effective oxide thickness and the resulting large capacitance cannot be achieved in conventional HfO 2 -based high-dielectric-constant gate stacks without scavenging the interfacial SiO 2 , which has adverse effects on the electron transport and gate leakage current. Accordingly, our gate stacks, which do not require such scavenging, provide substantially lower leakage current and no mobility degradation. This work demonstrates that ultrathin ferroic HfO 2 –ZrO 2 multilayers, stabilized with competing ferroelectric–antiferroelectric order in the two-nanometre-thickness regime, provide a path towards advanced gate oxide stacks in electronic devices beyond conventional HfO 2 -based high-dielectric-constant materials.

36 MATERIALS SCIENCE↗

700,000 years of tropical Andean glaciation

Our understanding of the climatic teleconnections that drove ice-age cycles has been limited by a paucity of well-dated tropical records of glaciation that span several glacial–interglacial intervals. Glacial deposits offer discrete snapshots of glacier extent but cannot provide the continuous records required for detailed interhemispheric comparisons. By contrast, lakes located within glaciated catchments can provide continuous archives of upstream glacial activity, but few such records extend beyond the last glacial cycle. Here a piston core from Lake Junín in the uppermost Amazon basin provides the first, to our knowledge, continuous, independently dated archive of tropical glaciation spanning 700,000 years. We find that tropical glaciers tracked changes in global ice volume and followed a clear approximately 100,000-year periodicity. An enhancement in the extent of tropical Andean glaciers relative to global ice volume occurred between 200,000 and 400,000 years ago, during sustained intervals of regionally elevated hydrologic balance that modified the regular approximately 23,000-year pacing of monsoon-driven precipitation. Millennial-scale variations in the extent of tropical Andean glaciers during the last glacial cycle were driven by variations in regional monsoon strength that were linked to temperature perturbations in Greenland ice cores; these interhemispheric connections may have existed during previous glacial cycles.

54 ENVIRONMENTAL SCIENCES↗

Ubiquitin-like conjugation by bacterial cGAS enhances anti-phage defence

Abstract cGAS is an evolutionarily conserved enzyme that has a pivotal role in immune defence against infection 1–3 . In vertebrate animals, cGAS is activated by DNA to produce cyclic GMP–AMP (cGAMP) 4,5 , which leads to the expression of antimicrobial genes 6,7 . In bacteria, cyclic dinucleotide (CDN)-based anti-phage signalling systems (CBASS) have been discovered 8–11 . These systems are composed of cGAS-like enzymes and various effector proteins that kill bacteria on phage infection, thereby stopping phage spread. Of the CBASS systems reported, approximately 39% contain Cap2 and Cap3 , which encode proteins with homology to ubiquitin conjugating (E1/E2) and deconjugating enzymes, respectively 8,12 . Although these proteins are required to prevent infection of some bacteriophages 8 , the mechanism by which the enzymatic activities exert an anti-phage effect is unknown. Here we show that Cap2 forms a thioester bond with the C-terminal glycine of cGAS and promotes conjugation of cGAS to target proteins in a process that resembles ubiquitin conjugation. The covalent conjugation of cGAS increases the production of cGAMP. Using a genetic screen, we found that the phage protein Vs.4 antagonized cGAS signalling by binding tightly to cGAMP (dissociation constant of approximately 30 nM) and sequestering it. A crystal structure of Vs.4 bound to cGAMP showed that Vs.4 formed a hexamer that was bound to three molecules of cGAMP. These results reveal a ubiquitin-like conjugation mechanism that regulates cGAS activity in bacteria and illustrates an arms race between bacteria and viruses through controlling CDN levels.

Science & Technology - Other Topics↗

Single-photon absorption and emission from a natural photosynthetic complex

Photosynthesis is generally assumed to be initiated by a single photon from the Sun, which, as a weak light source, delivers at most a few tens of photons per nanometre squared per second within a chlorophyll absorption band1. Yet much experimental and theoretical work over the past 40 years has explored the events during photosynthesis subsequent to absorption of light from intense, ultrashort laser pulses. Here, we use single photons to excite under ambient conditions the light-harvesting 2 (LH2) complex of the purple bacterium Rhodobacter sphaeroides, comprising B800 and B850 rings that contain 9 and 18 bacteriochlorophyll molecules, respectively. Excitation of the B800 ring leads to electronic energy transfer to the B850 ring in approximately 0.7 ps, followed by rapid B850-to-B850 energy transfer on an approximately 100-fs timescale and light emission at 850–875 nm. Using a heralded single photon source20,21 along with coincidence counting, we establish time correlation functions for B800 excitation and B850 fluorescence emission and demonstrate that both events involve single photons. We also find that the probability distribution of the number of heralds per detected fluorescence photon supports the view that a single photon can upon absorption drive the subsequent energy transfer and fluorescence emission and hence, by extension, the primary charge separation of photosynthesis. An analytical stochastic model and a Monte Carlo numerical model capture the data, further confirming that absorption of single photons is correlated with emission of single photons in a natural light-harvesting complex.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Integrated frequency-modulated optical parametric oscillator

Optical frequency combs have revolutionized precision measurement, time-keeping, and molecular spectroscopy. A substantial effort has developed around "microcombs": integrating comb-generating technologies into compact, reliable photonic platforms. Current approaches for generating these microcombs involve either the electro-optic (EO) or Kerr mechanisms. Despite rapid progress, maintaining high efficiency and wide bandwidth remains challenging. Here, we introduce a new class of microcomb -- an integrated optical frequency comb generator that combines electro-optics and parametric amplification to yield a frequency-modulated optical parametric oscillator (FM-OPO). In stark contrast to EO and Kerr combs, the FM-OPO microcomb does not form pulses but maintains operational simplicity and highly efficient pump power utilization with an output resembling a frequency-modulated laser. We outline the working principles of FM-OPO and demonstrate them by fabricating the complete optical system in thin-film lithium niobate (LNOI). We measure pump to comb internal conversion efficiency exceeding 93% (34% out-coupled) over a nearly flat-top spectral distribution spanning approximately 1,000 modes (approximately 6 THz). Compared to an EO comb, the cavity dispersion rather than loss determines the FM-OPO bandwidth, enabling broadband combs with a smaller RF modulation power. The FM-OPO microcomb, with its robust operational dynamics, high efficiency, and large bandwidth, contributes a new approach to the field of microcombs and promises to herald an era of miniaturized precision measurement, and spectroscopy tools to accelerate advancements in metrology, spectroscopy, telecommunications, sensing, and computing.

42 ENGINEERING↗

A high-density and high-confinement tokamak plasma regime for fusion energy

The tokamak approach, utilizing a toroidal magnetic field configuration to confine a hot plasma, is one of the most promising designs for developing reactors that can exploit nuclear fusion to generate electrical energy. To reach the goal of an economical reactor, most tokamak reactor designs simultaneously require reaching a plasma line-averaged density above an empirical limit—the so-called Greenwald density and attaining an energy confinement quality better than the standard high-confinement mode. However, such an operating regime has never been verified in experiments. In addition, a long-standing challenge in the high-confinement mode has been the compatibility between a high-performance core and avoiding large, transient edge perturbations that can cause very high heat loads on the plasma-facing-components in tokamaks. Here we report the demonstration of stable tokamak plasmas with a line-averaged density approximately 20% above the Greenwald density and an energy confinement quality of approximately 50% better than the standard high-confinement mode, which was realized by taking advantage of the enhanced suppression of turbulent transport granted by high density-gradients in the high-poloidal-beta scenario. Furthermore, our experimental results show an integration of very low edge transient perturbations with the high normalized density and confinement core. The operating regime we report supports some critical requirements in many fusion reactor designs all over the world and opens a potential avenue to an operating point for producing economically attractive fusion energy.

70 PLASMA PHYSICS AND FUSION TECHNOLOGY↗

Paclitaxel loading in cationic liposome vectors is enhanced by replacement of oleoyl with linoleoyl tails with distinct lipid shapes

Abstract Lipid carriers of hydrophobic paclitaxel (PTX) are used in clinical trials for cancer chemotherapy. Improving their loading capacity requires enhanced PTX solubilization. We compared the time-dependence of PTX membrane solubility as a function of PTX content in cationic liposomes (CLs) with lipid tails containing one (oleoyl; DOPC/DOTAP) or two (linoleoyl; DLinPC/newly synthesized DLinTAP) cis double bonds by using microscopy to generate kinetic phase diagrams. The DLin lipids displayed significantly increased PTX membrane solubility over DO lipids. Remarkably, 8 mol% PTX in DLinTAP/DLinPC CLs remained soluble for approximately as long as 3 mol% PTX (the solubility limit, which has been the focus of most previous studies and clinical trials) in DOTAP/DOPC CLs. The increase in solubility is likely caused by enhanced molecular affinity between lipid tails and PTX, rather than by the transition in membrane structure from bilayers to inverse cylindrical micelles observed with small-angle X-ray scattering. Importantly, the efficacy of PTX-loaded CLs against prostate cancer cells (their IC50 of PTX cytotoxicity) was unaffected by changing the lipid tails, and toxicity of the CL carrier was negligible. Moreover, efficacy was approximately doubled against melanoma cells for PTX-loaded DLinTAP/DLinPC over DOTAP/DOPC CLs. Our findings demonstrate the potential of chemical modifications of the lipid tails to increase the PTX membrane loading while maintaining (and in some cases even increasing) the efficacy of CLs. The increased PTX solubility will aid the development of liposomal PTX carriers that require significantly less lipid to deliver a given amount of PTX, reducing side effects and costs.

36 MATERIALS SCIENCE↗

Polyimide aerogels for ballistic impact protection

The ballistic performance of edge-clamped monolithic polyimide aerogel blocks (12 mm thickness) has been studied through a series of impact tests using a helium-filled gas gun connected to a vacuum chamber and a spherical steel projectile (approximately 3 mm diameter) with an impact velocity range of 150–1300 m s -1 . The aerogels had an average bulk density of 0.17 g cm -3 with high porosity of approximately 88%. The ballistic limit velocity of the aerogels was estimated to be in the range of 175–179 m s -1 . Moreover, the aerogels showed a robust ballistic energy absorption performance (e.g., at the impact velocity of 1283 m s -1 at least 18% of the impact energy was absorbed). At low impact velocities, the aerogels failed by ductile hole enlargement followed by a tensile failure. By contrast, at high impact velocities, the aerogels failed through an adiabatic shearing process. Given the substantially robust ballistic performance, the polyimide aerogels have a potential to combat multiple constraints such as cost, weight, and volume restrictions in aeronautical and aerospace applications with high blast resistance and ballistic performance requirements such as in stuffed Whipple shields for orbital debris containment application.

42 ENGINEERING↗

Mapping brucellosis risk in Kenya and its implications for control strategies in sub-Saharan Africa

In Sub-Saharan Africa (SSA), effective brucellosis control is limited, in part, by the lack of long-term commitments by governments to control the disease and the absence of reliable national human and livestock population-based data to inform policies. Therefore, we conducted a study to establish the national prevalence and develop a risk map for Brucella spp. in cattle to contribute to plans to eliminate the disease in Kenya by the year 2040. We randomly generated 268 geolocations and distributed them across Kenya, proportionate to the area of each of the five agroecological zones and the associated cattle population. Cattle herds closest to each selected geolocation were identified for sampling. Up to 25 cattle were sampled per geolocation and a semi-structured questionnaire was administered to their owners. We tested 6,593 cattle samples for Brucella immunoglobulin G (IgG) antibodies using an Enzyme-linked immunosorbent assay (ELISA). We assessed potential risk factors and performed spatial analyses and prevalence mapping using approximate Bayesian inference implemented via the integrated nested Laplace approximation (INLA) method. The national Brucella spp. prevalence was 6.8% (95% CI: 6.2–7.4%). Exposure levels varied significantly between agro-ecological zones, with a high of 8.5% in the very arid zone with the lowest agricultural potential relative to a low of 0.0% in the agro-alpine zone with the highest agricultural potential. Additionally, seroprevalence increased with herd size, and the odds of seropositivity were significantly higher for females and adult animals than for males or calves. Similarly, animals with a history of abortion, or with multiple reproductive syndromes had higher seropositivity than those without. At the herd level, the risk of Brucella spp. transmission was higher in larger herds, and herds with a history of reproductive problems such as abortion, giving birth to weak calves, or having swollen testes. Geographic localities with high Brucella seroprevalence occurred in northern, eastern, and southern regions of Kenya all primarily characterized by semi-arid or arid agro-ecological zones dominated by livestock pastoralism interspersed with vast areas with mixed livestock-wildlife systems. The large spatial extent of our survey provides compelling evidence for the widespread geographical distribution of brucellosis risk across Kenya in a manner easily understandable for policymakers. Our findings can provide a basis for risk-stratified pilot studies aiming to investigate the cost-effectiveness and efficacy of singular and combined preventive intervention strategies that seek to inform Kenya’s Brucellosis Control Policy.

60 APPLIED LIFE SCIENCES↗

VpROM: a novel variational autoencoder-boosted reduced order model for the treatment of parametric dependencies in nonlinear systems

Reduced Order Models (ROMs) are of considerable importance in many areas of engineering in which computational time presents difficulties. Established approaches employ projection-based reduction, such as Proper Orthogonal Decomposition. The limitation of the linear nature of such operators is typically tackled via a library of local reduction subspaces, which requires the assembly of numerous local ROMs to address parametric dependencies. Our work attempts to define a more generalisable mapping between parametric inputs and reduced bases for the purpose of generative modeling. We propose the use of Variational Autoencoders (VAEs) in place of the typically utilised clustering or interpolation operations, for inferring the fundamental vectors, termed as modes, which approximate the manifold of the model response for any and each parametric input state. The derived ROM still relies on projection bases, built on the basis of full-order model simulations, thus retaining the imprinted physical connotation. However, it additionally exploits a matrix of coefficients that relates each local sample response and dynamics to the global phenomena across the parametric input domain. The VAE scheme is utilised for approximating these coefficients for any input state. This coupling leads to a high-precision low-order representation, which is particularly suited for problems where model dependencies or excitation traits cause the dynamic behavior to span multiple response regimes. Moreover, the probabilistic treatment of the VAE representation allows for uncertainty quantification on the reduction bases, which may then be propagated to the ROM response. The performance of the proposed approach is validated on an open-source simulation benchmark featuring hysteresis and multi-parametric dependencies, and on a large-scale wind turbine tower characterised by nonlinear material behavior and model uncertainty.

Conditional VAEs↗

Uncertainty quantification in multivariable regression for material property prediction with Bayesian neural networks

With the increased use of data-driven approaches and machine learning-based methods in material science, the importance of reliable uncertainty quantification (UQ) of the predicted variables for informed decision-making cannot be overstated. UQ in material property prediction poses unique challenges, including multi-scale and multi-physics nature of materials, intricate interactions between numerous factors, limited availability of large curated datasets, etc. In this work, we introduce a physics-informed Bayesian Neural Networks (BNNs) approach for UQ, which integrates knowledge from governing laws in materials to guide the models toward physically consistent predictions. To evaluate the approach, we present case studies for predicting the creep rupture life of steel alloys. Experimental validation with three datasets of creep tests demonstrates that this method produces point predictions and uncertainty estimations that are competitive or exceed the performance of conventional UQ methods such as Gaussian Process Regression. Additionally, we evaluate the suitability of employing UQ in an active learning scenario and report competitive performance. The most promising framework for creep life prediction is BNNs based on Markov Chain Monte Carlo approximation of the posterior distribution of network parameters, as it provided more reliable results in comparison to BNNs based on variational inference approximation or related NNs with probabilistic outputs.

36 MATERIALS SCIENCE↗

Exploring the effects of molecular beam epitaxy growth characteristics on the temperature performance of state-of-the-art terahertz quantum cascade lasers

This study conducts a comparative analysis, using non-equilibrium Green’s functions (NEGF), of two state-of-the-art two-well (TW) Terahertz Quantum Cascade Lasers (THz QCLs) supporting clean 3-level systems. The devices have nearly identical parameters and the NEGF calculations with an abrupt-interface roughness height of 0.12 nm predict a maximum operating temperature (T max ) of ~ 250 K for both devices. However, experimentally, one device reaches a T max of ~ 250 K and the other a T max of only ~ 134 K. Both devices were fabricated and measured under identical conditions in the same laboratory, with high quality processes as verified by reference devices. The main difference between the two devices is that they were grown in different MBE reactors. Our NEGF-based analysis considered all parameters related to MBE growth, including the maximum estimated variation in aluminum content, growth rate, doping density, background doping, and abrupt-interface roughness height. From our NEGF calculations it is evident that the sole parameter to which a drastic drop in T max could be attributed is the abrupt-interface roughness height. We can also learn from the simulations that both devices exhibit high-quality interfaces, with one having an abrupt-interface roughness height of approximately an atomic layer and the other approximately a monolayer. However, these small differences in interface sharpness are the cause of the large performance discrepancy. This underscores the sensitivity of device performance to interface roughness and emphasizes its strategic role in achieving higher operating temperatures for THz QCLs. We suggest Atom Probe Tomography (APT) as a path to analyze and measure the (graded)-interfaces roughness (IFR) parameters for THz QCLs, and subsequently as a design tool for higher performance THz QCLs, as was done for mid-IR QCLs. Our study not only addresses challenges faced by other groups in reproducing the record T max of ~ 250 K and ~ 261 K but also proposes a systematic pathway for further improving the temperature performance of THz QCLs beyond the state-of-the-art.

77 NANOSCIENCE AND NANOTECHNOLOGY↗

Integration of multiple coinflip devices for high-quality random sampling

Artificial intelligence, scientific computing, and probabilistic computing use random sampling to approximate solutions to various problems, with larger models requiring a substantial quantity of random numbers. To generate the required vast quantity of random numbers at high rates, we explore so-called “coinflip” devices, which are stochastic microelectronic devices ideally capable of independently generating random bits with a tunable weight at a high rate. However, coinflip devices are inherently analog and demonstrate nonidealities, like temperature dependence and drift, that can introduce determinism into the outputs. We present important considerations for building systems of multiple coinflip devices to produce high-quality bitstreams with low error and little dependency on previous bits. Using tunnel diodes as coinflip devices, we implement a control loop to adapt to temperature dependence and generate fair bitstreams with each device. While this can lead to dependencies between bits in a single bitstream, we demonstrate that combining results generated in parallel with individual tunnel diodes can produce fair and unpredictable bitstreams. The suitability of these bitstreams for use in probabilistic computing is then demonstrated through a Monte Carlo approximation of π.

Taylor, Brady Garland [Sandia National Laboratorie↗

Multireference diffusion Monte Carlo reaches 2D materials

Abstract Quantum confinement in 2D materials strongly enhances electronic correlation effects. Therefore, predicting the properties of these unique materials, with both a high level of accuracy and computational efficiency, without relying on adjustable parameters or functionals, remains an outstanding theoretical challenge. The majority of theoretical studies are based on the approximations of density functional theory (DFT). The reliability of DFT predictions are heavily dependent on the choice of an approximated exchange-correlation functional. Here, we estimate the magnitude of impact of correlation on the total energy for the quintessential 2D material, graphene, by performing and comparing state-of-the-art selected CI and quantum Monte Carlo extrapolated calculations for a single unit cell at the$$\Gamma$$point. We demonstrate that Self-Healing Diffusion Monte Carlo (SHDMC) obtains a very compact, but high-quality wavefunction for this system that lacks the strong basis set dependence displayed by state of the art quantum chemistry methods. The SHDMC wavefunction is of higher quality compared to that obtained from sCI, in the same orbital basis, while being$$\sim$$ 1000 times smaller in terms of determinant count compared to sCI. We also demonstrate that extrapolating SHDMC results to the infinite determinant limit compares extremely well with complete basis set extrapolated sCI. Our work paves the way for future validation of SHDMC applied to challenging 2D materials.

Science & Technology - Other Topics↗

Upstreamness and downstreamness in input–output analysis from local and aggregate information

Abstract Ranking sectors and countries within global value chains is of paramount importance to estimate risks and forecast growth in large economies. However, this task is often non-trivial due to the lack of complete and accurate information on the flows of money and goods between sectors and countries, which are encoded in input–output (I–O) tables. In this work, we show that an accurate estimation of the role played by sectors and countries in supply chain networks can be achieved without full knowledge of the I–O tables, but only relying on local and aggregate information, e.g., the total intermediate demand per sector. Our method, based on a rank-1 approximation to the I–O table, shows consistently good performance in reconstructing rankings (i.e., upstreamness and downstreamness measures for countries and sectors) when tested on empirical data from the world input–output database. Moreover, we connect the accuracy of our approximate framework with the spectral properties of the I–O tables, which ordinarily exhibit relatively large spectral gaps. Our approach provides a fast and analytically tractable framework to rank constituents of a complex economy without the need of matrix inversions and the knowledge of finer intersectorial details.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗

Quantitative assessment of Ni + and He + ion irradiation damage in a tungsten heavy alloy under the simulated nuclear fusion environment

A 90W-7Ni-3Fe (wt.%) tungsten heavy alloy has been sequentially Ni + and He + ion irradiated at 700 °C to simulate the high temperature irradiation environment of a fusion reactor interior. W/Ni–Fe-W dual-phase alloys have been proposed to serve as plasma facing materials and require detailed investigation of their behavior under fusion relevant conditions to assess their overall applicability. To evaluate material performance under five years of simulated fusion reactor service, microstructural characterization of the nanoscale defect distribution has been performed on both constituent phases, revealing peak swelling in the W phase of approximately 0.03%. The γ-phase (Ni–Fe-W) is found to swell approximately 0.68% under the same irradiation conditions, indicating significant cavity formation and growth. Additionally, a novel multi-projection imaging approach has been applied to determine the extent of damage segregation along the dual-phase W-to-γ interface and exposes that these interfaces act as sink sites for the accumulation of cavities. Interphase boundaries are noted to possess an 11.8% areal coverage of defects along the boundary plane, primarily on the γ-phase side of the boundary. The accumulation of cavities at these interphase boundaries is anticipated to adversely affect overall material toughness, and this work reveals a pressing need for mechanical property testing of irradiated W–Ni-Fe dual-phase alloys.

70 PLASMA PHYSICS AND FUSION TECHNOLOGY↗

Coupled electronic and magnetic excitations in the cuprates and their role in the superconducting transition

The formation of Cooper pairs, a bound state of two electrons of opposite spin and momenta by exchange of a phonon, is a defining feature of conventional superconductivity. In the cuprate high temperature superconductors, even though the superconducting state also consists of Cooper pairs, the pairing mechanism remains intensely debated. Here, we investigate superconducting pairing in the Bi 2 Sr 2 CaCu 2 O 8+δ (Bi2212) cuprate by employing spectral functions obtained from angle-resolved photoemission as input to the Bethe-Salpeter equation. Assuming Cooper pairing is driven by spin fluctuations, we construct the spin-fluctuation-mediated pairing interaction and use it to compute the eigenfunctions and eigenvalues of the Bethe-Salpeter equation for multiple Bi2212 samples. The leading d-wave eigenvalue increases as the temperature is decreased toward $T_c$, reaching a value of approximately 1 at the $T_c$ corresponding to each doping value. This suggests that spin fluctuations can approximately account for $T_c$ and mediate pairing in the cuprate superconductors.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗

Quantifying the hydration structure of sodium and potassium ions: taking additional steps on Jacob's Ladder

The ability to reproduce the experimental structure of water around the sodium and potassium ions is a key test of the quality of interaction potentials due to the central importance of these ions in a wide range of important phenomena. In this study, we simulate the Na + and K + ions in bulk water using three density functional theory functionals: (1) the generalized gradient approximation (GGA) based dispersion corrected revised Perdew, Burke, and Ernzerhof functional (revPBE-D3) (2) the recently developed strongly constrained and appropriately normed (SCAN) functional (3) the random phase approximation (RPA) functional for potassium. We compare with experimental X-ray diffraction (XRD) and X-ray absorption fine structure (EXAFS) measurements to demonstrate that SCAN accurately reproduces key structural details of the hydration structure around the sodium and potassium cations, whereas revPBE-D3 fails to do so. However, we show that SCAN provides a worse description of pure water in comparison with revPBE-D3. RPA also shows an improvement for K + , but slow convergence prevents rigorous comparison. Finally, we analyse cluster energetics to show SCAN and RPA have smaller fluctuations of the mean error of ion–water cluster binding energies compared with revPBE-D3.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗