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Search indexed NASA NTRS and DOE OSTI research on propulsion, heat transfer, battery materials and energy systems. Follow report and document links to the original sources.

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All sourcesNASA NTRSDOE OSTI
NASA NTRS2002

Evidence of an Intrinsic Intraseasonal Oscillation over Tropical South America During Austral Summer

The intraseasonal variation (ISV) in the 30-60 day band, also known as Madden-Julian oscillation (MJO), has been studied for decades. Madden and Julian showed that the oscillation originated from the western Indian Ocean, propagated eastward, got enhanced over the maritime continent and weakened after passing over the dateline. Composite studies showed evidences of a signal in upper and lower level zonal wind propagating around the globe during an oscillation. Theoretical studies pointed out that the interaction with the warm ocean surface and the coupling with the convective and radiative processes in the atmosphere could manifest the oscillation, which propagates eastward via mutual feedbacks between the wave motions and the cumulus heating. Over tropical South America, no independent 30-60 day oscillation has been reported so far, despite that Amazon is the most distinct tropical convection center over the western hemisphere and the fluxes from its surface of tropical rainforests are close to that from the warm tropical ocean. Liebmann et al. showed a distinct spectral peak of 40-50 day oscillation in outgoing longwave radiation (OLR) over tropical South America and considered that was manifested by the MJO propagation. Nogues-Paegle et al. (2000) focused on a dipole pattern of the OLR anomaly with centers of action over the South Atlantic Convergence Zone (SACZ) and the subtropical plain. They used the regional 10-90 day filtered data and demonstrated this pattern could be represented by the fifth mode of the rotated empirical orthogonal function. Its principal component was further analyzed using the singular spectrum analysis. Their result showed two oscillatory modes with periods of 36-40 days and 22-28 days, of which the former was related to the MJO influence and the latter linked to the remote forcing over southwest of Australia, which produced a wave train propagating southeastward, rounding the southern tip of South America and returning back toward the northeast. The 22-28 day mode has distinct impact on SACZ, responsible for the regional seesaw pattern of alternating dry and wet conditions. In this study we will focus on the 30-60-day spectral band and investigate whether the independent oscillation source over tropical South America is existed. First, we will show the seasonal dependence of the tropical South American ISV in Section 3. Then, the leading principal modes of 30-60 day bandpass filtered 850-hPa velocity potential (VP850) will be computed to distinguish the stationary ISV over tropical South America (SISA) from the propagating MJO in the austral summertime in Section 4. The importance of SISA in representing the regional ISV over South America will be discussed. In Section 5, we will demonstrate the mass oscillation regime of SISA, which is well separated from that of MJO by the Andes, and the convective coupling with rainfall. The dynamical response of SISA and the impact on the South American summer monsoon (SASM) will be presented. Finally, we will give the concluding remarks.

Zhou, Jiayu↗
DOE OSTI2024

Integrable symplectic maps with a polygon tessellation

Identifying integrable dynamics remains a formidable challenge, and despite centuries of research, only a handful of examples are known to date. In this article, we explore a distinct form of area-preserving (symplectic) mappings derived from the stroboscopic Poincaré cross section of a kicked rotator—an oscillator subjected to an external force periodically switched on in short pulses. The significance of this class of problems extends to various applications in physics and mathematics, including particle accelerators, crystallography, and studies of chaos. Notably, Suris's theorem constrains the integrability within this category of mappings, outlining potential scenarios with analytic invariants of motion. In this paper, we challenge the assumption of the analyticity of the invariant by exploring piecewise linear transformations on a torus ( T 2 ) and associated systems on the plane ( R 2 ), incorporating arithmetic quasiperiodicity and discontinuities. Introducing a new automated technique, we discovered previously unknown scenarios featuring polygonal invariants that form perfect tessellations and, moreover, fibrations of the plane or torus. This work reveals a novel category of planar tilings characterized by discrete symmetries that emerge from the invertibility of transformations and are intrinsically linked to the presence of integrability. Our algorithm relies on the analysis of the Poincaré rotation number and its piecewise monotonic nature for integrable cases, contrasting with the noisy behavior in the case of chaos, thereby allowing for clear separation. Some of the newly discovered systems exhibit the peculiar behavior of “integrable diffusion,” characterized by infinite and quasirandom hopping between tiles while being confined to a set of invariant segments. Finally, through the implementation of a smoothening procedure, all mappings can be generalized to quasi-integrable scenarios with suppressed volume occupied by chaotic trajectories, thereby opening doors to potential practical applications. Published by the American Physical Society 2024

43 PARTICLE ACCELERATORS↗
NASA NTRS1995

Galactic oscillator symmetry

Riemann ellipsoids model rotating galaxies when the galactic velocity field is a linear function of the Cartesian coordinates of the galactic masses. In nuclear physics, the kinetic energy in the linear velocity field approximation is known as the collective kinetic energy. But, the linear approximation neglects intrinsic degrees of freedom associated with nonlinear velocity fields. To remove this limitation, the theory of symplectic dynamical symmetry is developed for classical systems. A classical phase space for a self-gravitating symplectic system is a co-adjoint orbit of the noncompact group SP(3,R). The degenerate co-adjoint orbit is the 12 dimensional homogeneous space Sp(3,R)/U(3), where the maximal compact subgroup U(3) is the symmetry group of the harmonic oscillator. The Hamiltonian equations of motion on each orbit form a Lax system X = (X,F), where X and F are elements of the symplectic Lie algebra. The elements of the matrix X are the generators of the symplectic Lie algebra, viz., the one-body collective quadratic functions of the positions and momenta of the galactic masses. The matrix F is composed from the self-gravitating potential energy, the angular velocity, and the hydostatic pressure. Solutions to the hamiltonian dynamical system on Sp(3,R)/U(3) are given by symplectic isospectral deformations. The Casimirs of Sp(3,R), equal to the traces of powers of X, are conserved quantities.

Rosensteel, George↗
DOE OSTI2025

CryoDRGN-AI: neural ab initio reconstruction of challenging cryo-EM and cryo-ET datasets

Proteins and other biomolecules form dynamic macromolecular machines that are tightly orchestrated to move, bind, and perform chemistry. Cryo-electron microscopy (cryo-EM) and cryo-electron tomography (cryo-ET) can access the intrinsic heterogeneity of these complexes and are therefore key tools for understanding their function. However, 3D reconstruction of the collected imaging data presents a challenging computational problem, especially without any starting information, a setting termed ab initio reconstruction. Here, in this study, we introduce cryoDRGN-AI, a method leveraging an expressive neural representation and combining an exhaustive search strategy with gradient-based optimization to process challenging heterogeneous datasets. Using cryoDRGN-AI, we reveal new conformational states in large datasets, reconstruct previously unresolved motions from unfiltered datasets, and demonstrate ab initio reconstruction of biomolecular complexes from in situ data. With this expressive and scalable model for structure determination, we hope to unlock the full potential of cryo-EM and cryo-ET as a high-throughput tool for structural biology and discovery.

Levy, Axel [Stanford Univ., CA (United States); SL↗
NASA NTRS1991

Solar wind dynamic pressure variations and possible ground signatures of flux transfer events

The effects of a series of solar wind dynamic pressure pulses are followed through the solar wind, across the bow shock and magnetosheath, into the magnetosphere, and down to the dayside ionosphere. Each pressure pulse had an intrinsic solar wind origin, i.e., was not generated by processes occurring at the earth's bow shock. Both upstream and downstream of the earth's bow shock, the pulses were identified by depressed magnetic field strengths and enhanced plasma densities. The pulses compressed the magnetosheath and magnetosphere, causing satellites in the magnetosphere to briefly observe enhanced magnetic field strengths, and/or enter the low-latitude boundary layer or magnetosheath. Satellites already in the magnetosheath observed a brief burst of enhanced magnetosheath flow caused by the relative inward motion of magnetosheath flow patterns. Alfven and fast mode compressional waves propagated rapidly down to the polar ionosphere, where they produced transient ionospheric flows at latitudes equatorward of the convection reversal boundary. The flow patterns moved westward around the auroral oval.

Sibeck, D. G.↗
NASA NTRS2022

The International DORIS Service contribution to ITRF2020

For the realization of the 2020 International Terrestrial Reference Frame (ITRF2020), the International DORIS Service delivered to the International Earth Rotation and Reference Systems Service (IERS) a set of 1456 weekly solution files from 1993.0 to 2021.0 including station coordinates and Earth orientation parameters (EOPs). The data come from fourteen DORIS satellites: TOPEX/Poseidon, SPOT-2, SPOT-3, SPOT-4, SPOT-5, Envisat, Jason-1, Jason-2, Cryosat-2, Saral, HY-2A, Jason-3, Sentinel-3A and Sentinel-3B. In their processing, the four analysis centers which contributed to the DORIS combined solution used the latest time variable gravity models, the new mean pole and diurnal-subdiurnal tidal EOP models recommended by IERS. In addition, all the analysis centers included in their processing precise SPOT-5 solar panel angle values and quaternions for, at least, the Jason satellites. Furthermore, a new Alcatel phase center variation model was implemented for the ITRF2020 processing. The main objective of this study is to present the combination process and to analyze the impact of the new modeling on the performance of the new combined solution. Comparisons with the IDS contribution to ITRF2014 show that i) the application of the new phase center variations for the Alcatel DORIS ground antennas in the data processing combined with the gradual replacement over time of the Alcatel by Starec antennas implies a scale drift from 1993.0 to 2002.5 and ii) thanks to a better modeling of the surface forces on the satellites, the new combined solution shows smaller annual and 118-day signals in the geocenter. A new DORIS terrestrial reference frame was computed to evaluate the intrinsic quality of the new combined solution. That evaluation shows that over almost the full time span the intrinsic IDS scale values lie in a range of ±5 mm. After mid-2008, the new DORIS reference frame has an internal position consistency in North-East-Up better than 7.5 mm.

DORIS↗
NASA NTRS1997

Kinematics and M(sub v) calibration of K and M dwarf stars using Hipparcos data

The luminosities and kinematics of lower main sequence stars in a spectroscopically selected sample covering spectral types K 3 to M 5 are determined using Hipparcos parallaxes and proper motions. The stars separate into two kinematically distinct components, called young disk and old disk components. The young component has velocity dispersion (30, 17, 12) km/s in the U, V and W directions, respectively, and features an asymmetric drift of 8 km/s, a vertex deviation of 10 +/- 3 deg and an absolute magnitude of 10.48 mag at color (R - I)(sub Kron) = 1.0 mag. The respective features of the old component are: (56, 34, 31) km/s, 28 km/s and 0.6 mag at the same color. The slope and intrinsic width of the magnitude calibration of each component are determined. The analysis is used to investigate the possible presence of residual systematic discrepancies of the model with Hipparcos data. There are indications of a possible underestimation of the parallax errors.

Upgren, A. R.↗
DOE OSTI2022

Solutal-buoyancy-driven intertwining and rotation of patterned elastic sheets

Abstract The intertwining of strands into 3D spirals is ubiquitous in biology, enabling functions from information storage to maintenance of cell structure and directed locomotion. In synthetic systems, entwined fibers can provide superior mechanical properties and act as artificial muscle or structural reinforcements. Unlike structures in nature, the entwinement of synthetic materials typically requires application of an external stimulus, such as mechanical actuation, light, or a magnetic field. Herein, we use computational modeling to design microscale sheets that mimic biology by transducing chemical energy into mechanical action, and thereby self-organize and interlink into 3D spirals, which spontaneously rotate. These flexible sheets are immersed in a fluid-filled microchamber that encompasses an immobilized patch of catalysts on the bottom wall. The sheets themselves can be passive or active (coated with catalyst). Catalytic reactions in the solution generate products that occupy different volumes than the reactants. The resulting density variations exert a force on the fluid (solutal buoyancy force) that causes motion, which in turn drives the interlinking and collective swirling of the sheets. The individual sheets do not rotate; rotation only occurs when the sheets are interlinked. This level of autonomous, coordinated 3D structural organization, intertwining, and rotation is unexpected in synthetic materials systems operating without external controls. Using physical arguments, we identify dimensionless ratios that are useful in scaling these ideas to other systems. These findings are valuable for creating materials that act as “machines”, and directing soft matter to undergo self-sustained, multistep assembly that is governed by intrinsic chemical reactions.

Manna, Raj Kumar (ORCID:0000000322729487)↗
NASA NTRS1972

Space and time variations of the solar Na D line profiles.

Preliminary results are presented of observations of the solar Na D lines obtained with high space and time resolution. The line profiles vary strongly with space and time implying that time averaging over a long period and large area will not produce the 'true' profile. The centre-limb increase in apparent Doppler width in the D lines is intrinsic. It is not due to space or time averaging. The amplitude of the 300-sec oscillation may range up to 1.5 km/sec in the region of formation of the D lines. The variation of the D line profile caused by the 300-sec oscillation may be described as follows: (1) the core is raised and lowered without change of shape, and (2) the wings broaden as the central intensity rises and narrow as it falls. Doppler width values derived from pairs of D line profiles are strongly correlated with the motion of the element observed. Indications of running waves have been found in the time variation of the core line bisectors.

Slaughter, C. D.↗
DOE OSTI2020

Accurate prediction of core-level spectra of radicals at density functional theory cost via square gradient minimization and recoupling of mixed configurations

State-specific orbital optimized approaches are more accurate at predicting core-level spectra than traditional linear-response protocols, but their utility had been restricted due to the risk of "variational collapse" down to the ground state. We employ the recently developed square gradient minimization algorithm to reliably avoid variational collapse and study the effectiveness of orbital optimized density functional theory (DFT) at predicting second period element 1s core-level spectra of open-shell systems. Several density functionals (including SCAN, B3LYP, and ωB97X-D3) are found to predict excitation energies from the core to singly occupied levels with high accuracy (≤0.3 eV RMS error) against available experimental data. Higher excited states are, however, more challenging by virtue of being intrinsically multiconfigurational. We thus present a configuration interaction inspired route to self-consistently recouple single determinant mixed configurations obtained from DFT, in order to obtain approximate doublet states. This recoupling scheme is used to predict the C K-edge spectra of the allyl radical, the O K-edge spectra of CO + , and the N K-edge of NO 2 with high accuracy relative to experiment, indicating substantial promise in using this approach for the computation of core-level spectra for doublet species [vs more traditional time dependent DFT, equation of motion coupled cluster singles and doubles (EOM-CCSD), or using unrecoupled mixed configurations]. Finally, we also present general guidelines for computing core-excited states from orbital optimized DFT.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2020

Charging-driven coarsening and melting of a colloidal nanoparticle monolayer at an ionic liquid–vacuum interface

In this work, we induce and investigate the coarsening and melting dynamics of an initially static nanoparticle colloidal monolayer at an ionic liquid–vacuum interface, driven by a focused, scanning electron beam. Coarsening occurs through grain interface migration and larger-scale motions such as grain rotations, often facilitated by sliding dislocations. The progressive decrease in area fraction that drives melting of the monolayer is explained using an electrowetting model whereby particles at the interface are solvated once their accumulating charge recruits sufficient counterions to subsume the particle. Subject to stochastic particle removal from the monolayer, melting is recapitulated in simulations with a Lennard-Jones potential. This new driving mechanism for colloidal systems, whose dynamical timescales we show can be controlled with the accelerating voltage, opens the possibility to manipulate particle interactions dynamically without need to vary particle intrinsic properties or surface treatments. Furthermore, the decrease in particle size availed by electron imaging presents opportunities to observe force and time scales in a lesser-explored regime intermediate between typical colloidal and molecular systems.

36 MATERIALS SCIENCE↗
DOE OSTI2021

Effects of magnetic fields on HPGe tracking detectors

Here, we present a study of magnetic fields effects on the position resolution and energy response of hyper-pure germanium detectors. Our results provide realistic estimates of the potential impact on the resolving power of tracking-arrays from (fringe) magnetic fields present when operating together with large spectrometers. By solving the equations of motion for the electron and holes in the presence of both electric and magnetic fields, we analyzed the drift trajectories of the charge carriers to determine the deviations in the positions at the end point of the trajectories, as well as changes in drift lengths affecting the energy resolution and peak shift due to trapping. Our results show that the major effect is in the deviation of the transverse (to the electric field direction) position and suggest that, if no corrective action is taken in the pulse-shape and tracking data analysis procedures, a field strength ≳ 0.1 T will start to impact the intrinsic position resolution of 2 mm (RMS). At fields above ~1 T, the degradation of the energy response becomes observable.

46 INSTRUMENTATION RELATED TO NUCLEAR SCIENCE AND ↗
DOE OSTI2019

Progress towards a phenomenological picture and theoretical understanding of glassy dynamics and vitrification near interfaces and under nanoconfinement

The nature of alterations to dynamics and vitrification in the nanoscale vicinity of interfaces-commonly referred to as "nanoconfinement" effects on the glass transition-has been an open question for a quarter century. We first analyze experimental and simulation results over the last decade to construct an overall phenomenological picture. Key features include the following: after a metrology- and chemistry-dependent onset, near-interface relaxation times obey a fractional power law decoupling relation with bulk relaxation; relaxation times vary in a double-exponential manner with distance from the interface, with an intrinsic dynamical length scale appearing to saturate at low temperatures; the activation barrier and vitrification temperature T-g approach bulk behavior in a spatially exponential manner; and all these behaviors depend quantitatively on the nature of the interface. We demonstrate that the thickness dependence of film-averaged T-g for individual systems provides a poor basis for discrimination between different theories, and thus we assess their merits based on the above dynamical gradient properties. Entropy-based theories appear to exhibit significant inconsistencies with the phenomenology. Diverse free-volume-motivated theories vary in their agreement with observations, with approaches invoking cooperative motion exhibiting the most promise. The elastically cooperative nonlinear Langevin equation theory appears to capture the largest portion of the phenomenology, although important aspects remain to be addressed. A full theoretical understanding requires improved confrontation with simulations and experiments that probe spatially heterogeneous dynamics within the accessible 1-ps to 1-year time window, minimal use of adjustable parameters, and recognition of the rich quantitative dependence on chemistry and interface. Published under license by AIP Publishing.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
NASA NTRS2001

Microphysics, Meteorology, Microwave and Modeling of Mediterranean Storms: The M(sup 5) Problem

Comprehensive understanding of the microphysical nature of Mediterranean storms requires a combination of in situ meteorological data analysis and radar-passive microwave data analysis, effectively integrated with numerical modeling studies at various scales, particularly from synoptic scale down to mesoscale. The microphysical properties of and their controls on severe storms are intrinsically related to meteorological processes under which storms have evolved, processes which eventually select and control the dominant microphysical properties themselves. Insofar as hazardous Mediterranean storms, highlighted by the September 25-28/1992 Genova flood event, the October 5-7/1998 Friuli flood event, and the October 13-15/2000 Piemonte flood event (all taking place in northern Italy), developing a comprehensive microphysical interpretation requires an understanding of the multiple phases of storm evolution and the heterogeneous nature of precipitation fields within the storm domains. This involves convective development, stratiform transition and decay, orographic lifting, and sloped frontal lifting proc esses. This also involves vertical motions and thermodynamical instabilities governing physical processes that determine details of the liquid/ice water contents, size distributions, and fall rates of the various modes of hydrometeors found within the storm environments. This paper presents detailed 4-dimensional analyses of the microphysical elements of the three severe Mediterranean storms identified above, investigated with the aid of SSM/I and TRMM satellite measurements (and other remote sensing measurements). The analyses are guided by nonhydrostatic mesoscale model simulations at high resolution of the intense rain producing portions of the storm environments. The results emphasize how meteorological controls taking place at the large scale, coupled with localized terrain controls, ultimately determine the most salient features of the bulk microphysical properties of the storms. These results have bearing on precipitation remote sensing from space, and the role of modeling in designing precipitation retrieval algorithms.

Smith, Eric A.↗
NASA NTRS2001

Predictive Compensator Optimization for Head Tracking Lag in Virtual Environments

We examined the perceptual impact of plant noise parameterization for Kalman Filter predictive compensation of time delays intrinsic to head tracked virtual environments (VEs). Subjects were tested in their ability to discriminate between the VE system's minimum latency and conditions in which artificially added latency was then predictively compensated back to the system minimum. Two head tracking predictors were parameterized off-line according to cost functions that minimized prediction errors in (1) rotation, and (2) rotation projected into translational displacement with emphasis on higher frequency human operator noise. These predictors were compared with a parameterization obtained from the VE literature for cost function (1). Results from 12 subjects showed that both parameterization type and amount of compensated latency affected discrimination. Analysis of the head motion used in the parameterizations and the subsequent discriminability results suggest that higher frequency predictor artifacts are contributory cues for discriminating the presence of predictive compensation.

Adelstein, Barnard D.↗
DOE OSTI2024

Chlorophyll to zeaxanthin energy transfer in nonphotochemical quenching: An exciton annihilation-free transient absorption study

Zeaxanthin (Zea) is a key component in the energy-dependent, rapidly reversible, nonphotochemical quenching process (qE) that regulates photosynthetic light harvesting. Previous transient absorption (TA) studies suggested that Zea can participate in direct quenching via chlorophyll (Chl) to Zea energy transfer. However, the contamination of intrinsic exciton–exciton annihilation (EEA) makes the assignment of TA signal ambiguous. In this study, we present EEA-free TA data using Nicotiana benthamiana thylakoid membranes, including the wild type and three NPQ mutants (npq1, npq4, and lut2) generated by CRISPR/Cas9 mutagenesis. The results show a strong correlation between excitation energy transfer from excited Chl Q y to Zea S 1 and the xanthophyll cycle during qE activation. Notably, a Lut S 1 signal is absent in the npq1 thylakoids which lack zeaxanthin. Additionally, the fifth-order response analysis shows a reduction in the exciton diffusion length (L D ) from 62 ± 6 nm to 43 ± 3 nm under high light illumination, consistent with the reduced range of exciton motion being a key aspect of plants’ response to excess light.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
NASA NTRS1991

Rotational properties of planetary satellites

Properties of satellite rotation that are observable in principle, include the rotation period, the orientation of the spin axis relative to the orbit plane, precession of the spin axis due to gravitational torques, nonprincipal axis rotation or wobble, and deviations from uniform principle axis rotation or libration. Considerable order is observed in current satellite rotation states, and it is of interest to ascertain how this order came about and why some satellites do not conform to the dominant norm. There is a strong coupling between the spin and orbital motions that is primarily responsible for maintaining the ordered rotation states in most cases, but this coupling is equally responsible for destroying any chance of orderly rotation for Saturn's satellite Hyperion. Understanding the processes which constrain current rotation states as well as those of an evolutionary nature which could have brought the individual satellites to their observed rotation and orbit states allows us to sometimes infer interior properties of some satellite or even of its primary planet, although, attempts to deduce primordial rotation states are usually frustrated. The observed rotational properties of the planetary satellites are summarized, and the understanding of the processes maintaining and those leading to the observed states are outlined. Some of the inferences that can be drawn about intrinsic properties of the bodies themselves are indicated.

Peale, S. J.↗
DOE OSTI2021

Toward a First-Principles Framework for Predicting Collective Properties of Electrolytes

Conspectus Given the universal importance of electrolyte solutions, it is natural to expect that we have a nearly complete understanding of the fundamental properties of these solutions (e.g., the chemical potential) and that we can therefore explain, predict, and control the phenomena occurring in them. In fact, reality falls short of these expectations. But, recent advances in the simulation and modeling of electrolyte solutions indicate that it should soon be possible to make progress toward these goals. In this Account, we will discuss the use of first-principles interaction potentials based in quantum mechanics (QM) to enhance our understanding of electrolyte solutions. Specifically, we will focus on the use of quantum density functional theory (DFT) combined with molecular dynamics simulation (DFT-MD) as the foundation for our approach. The overarching concept is to understand and accurately reproduce the balance between local or short-ranged (SR) structural details and long-range (LR) correlations, allowing the prediction of the thermodynamics of both single ions in solution as well as the collective interactions characterized by activity/osmotic coefficients. In doing so, relevant collective motions and driving forces characterized by chemical potentials can be determined. Here, in this Account, we will make the case that understanding electrolyte solutions requires a faithful QM representation of the SR nature of the ion–ion, ion–water, and water–water interactions. However, the number of molecules that is required for collective behavior makes the direct application of high-level QM methods that contain the best SR physics untenable, making methods that balance accuracy and efficiency a practical goal. Alternatives such as continuum solvent models (CSMs) and empirically based classical molecular dynamics have been extensively employed to resolve this problem but without yet overcoming the fundamental issue of SR accuracy. We will demonstrate that accurately describing the SR interaction is imperative for predicting both intrinsic properties, namely, at infinite dilution, and collective properties of electrolyte solutions. DFT has played an important role in our understanding of condensed phase systems, e.g., bulk liquid water, the air–water interface, ions in bulk, and at the air–water interface. This approach holds huge promise to provide benchmark calculations of electrolyte solution properties that will allow for the development and improvement of more efficient methods, as well as an enhanced understanding of fundamental phenomena. However, the standard protocol using the generalized gradient approximation with van der Waals (vdW) correction requires improvement in order to achieve a high level of quantitative accuracy. Simply simulating with higher level DFT functionals may not be the best route considering the significant computational cost. Alternative methods of incorporating information from higher levels of QM should be explored; e.g., using force matching techniques on small clusters, where high level benchmark calculations are possible, to develop ideal correction terms to the DFT functional is a promising possibility. We argue that DFT with statistical mechanics is becoming an increasingly useful framework enabling the prediction of collective electrolyte properties.

Duignan, Timothy T.↗