Results for “transitivity” — Page 19

DOE OSTI2023

Constraints on a split superconducting transition under uniaxial strain in Sr 2 RuO 4 from scanning SQUID microscopy

More than two decades after the discovery of superconductivity in Sr 2 RuO 4 , it is still unclear whether the order parameter has a single component or two degenerate components. For any two-component scenario, application of uniaxial strain is expected to lift the degeneracy, generating two distinct phase transitions. The presence of a second (lower-temperature) transition may be observable by probes that are sensitive to changes in the London penetration depth, λ, as a function of temperature, T. Furthermore, we use scanning SQUID microscopy combined with a uniaxial strain device to test for a second transition under strain. We only observe a single transition. Within the temperature range where a second transition has been suggested by μSR measurements, we further place a tight upper bound of less than 1% on the change in the zero temperature superfluid density n s ∝ λ –2 (0) due to a second transition, suggesting that such a transition does not occur. These results constrain theories of the order parameter in Sr 2 RuO 4 .

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗

DOE OSTI2022

Zero Magnetic Field Plateau Phase Transition in Higher Chern Number Quantum Anomalous Hall Insulators

The plateau-to-plateau transition in quantum Hall effect under high magnetic fields is a celebrated quantum phase transition between two topological states. It can be achieved by either sweeping the magnetic field or tuning the carrier density. The recent realization of the quantum anomalous Hall (QAH) insulators with tunable Chern numbers introduces the channel degree of freedom to the dissipation-free chiral edge transport and makes the study of the quantum phase transition between two topological states under zero magnetic field possible. Here, we synthesized the magnetic topological insulator (TI)/TI pentalayer heterostructures with different Cr doping concentrations in the middle magnetic TI layers using molecular beam epitaxy. By performing transport measurements, we found a potential plateau phase transition between C=1 and C=2 QAH states under zero magnetic field. In tuning the transition, the Hall resistance monotonically decreases from h/e2 to h/2e 2 , concurrently, the longitudinal resistance exhibits a maximum at the critical point. Our results show that the ratio between the Hall resistance and the longitudinal resistance is greater than 1 at the critical point, which indicates that the original chiral edge channel from the C=1 QAH state coexists with the dissipative bulk conduction channels. Subsequently, these bulk conduction channels appear to self-organize and form the second chiral edge channel in completing the plateau phase transition. Our study will motivate further investigations of this novel Chern number change-induced quantum phase transition and advance the development of the QAH chiral edge current-based electronic and spintronic devices.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗

DOE OSTI2023

Study of Seamless Microgrid Transition Operation Using Grid-Forming Inverters

This paper investigates operational techniques to achieve seamless (smooth) microgrid (MG) transitions by dispatching a grid-forming (GFM) inverter. In traditional approaches, the GFM inverter must switch between grid-following (GFL) and GFM control modes during MG transition operation. Today's inverter technology allows GFM inverters to always operate in GFM control mode, so it is worth exploring how to use them to achieve smooth MG transition operation. This paper proposes three operational techniques: a traditional scheme of switching between GFL and GFM control; a new scheme of consistent GFM control and shifting the droop intercept up before islanding operation; and a new scheme of consistent GFM control and shifting the droop intercept up before synchronization operation. A full hardware setup is established to compare the three techniques and showcase their implementations in real-world applications. The results show that the third technique outperforms the others and exhibits the best transition performance because the GFM inverter maintains the same operating points during the transition operation. Therefore, we conclude that ensuring smooth MG transition operation requires that the GFM inverter(s) maintain the same operating points (v, f, P, Q, and phase angle) during the transition operation in addition to minimizes the point of common coupling power flow.

grid-forming control↗

DOE OSTI2021

Machine Learning Predictions of Transition Probabilities in Atomic Spectra

Forward modeling of optical spectra with absolute radiometric intensities requires knowledge of the individual transition probabilities for every transition in the spectrum. In many cases, these transition probabilities, or Einstein A-coefficients, quickly become practically impossible to obtain through either theoretical or experimental methods. Complicated electronic orbitals with higher order effects will reduce the accuracy of theoretical models. Experimental measurements can be prohibitively expensive and are rarely comprehensive due to physical constraints and sheer volume of required measurements. Due to these limitations, spectral predictions for many element transitions are not attainable. In this work, we investigate the efficacy of using machine learning models, specifically fully connected neural networks (FCNN), to predict Einstein A-coefficients using data from the NIST Atomic Spectra Database. For simple elements where closed form quantum calculations are possible, the data-driven modeling workflow performs well but can still have lower precision than theoretical calculations. For more complicated nuclei, deep learning emerged more comparable to theoretical predictions, such as Hartree–Fock. Unlike experiment or theory, the deep learning approach scales favorably with the number of transitions in a spectrum, especially if the transition probabilities are distributed across a wide range of values. It is also capable of being trained on both theoretical and experimental values simultaneously. In addition, the model performance improves when training on multiple elements prior to testing. The scalability of the machine learning approach makes it a potentially promising technique for estimating transition probabilities in previously inaccessible regions of the spectral and thermal domains on a significantly reduced timeline.

74 ATOMIC AND MOLECULAR PHYSICS↗

NASA NTRS2020

Tuning Neural Network Models for Improved Prediction of Boundary Layer Transition

Boundary layer transition can strongly impact flight vehicle performance as it influences surface skin friction and aerodynamic heating, making accurate transition prediction a key to designing next generation aircraft. Artificial neural networks (ANNs) have shown promise toward predicting laminar-turbulent transition based on linear stability correlations. The computational efficiency of ANNs and the substantially reduced user involvement in relation to direct computations based on the linear stability theory (LST) makes them an attractive methodology for integrating the LST based correlations in computational fluid dynamics codes. Tollmien-Schlichting (TS) waves correspond to the dominant transition mechanism in 2D or weakly 3D subsonic boundary layers, such as those encountered in general aviation applications. Improvements to neural network model accuracy in predicting the amplification rates of TS instability waves have been investigated by leveraging recent machine learning developments in conjunction with surrogate optimization techniques and via suitable augmentation of the data used to train the networks. The optimized models trained on the modified dataset reduced the average transition location errors on different airfoils at several flow conditions by 51% of the original manually-tuned network’s errors on the same flow cases. The actual transition locations were derived from the Langley Stability and Transition Analysis Code (LASTRAC).

Machine Learning↗

NASA NTRS2021

Transition Analysis for the CRM-NLF Wind Tunnel Configuration

This paper presents the results of an ongoing study into the linear stability characteristics of the boundary layer flow over the common research model with natural laminar flow (CRMNLF) aircraft configuration. The flow conditions match selected test conditions from a recent wind tunnel experiment in the National Transonic Facility at the NASA Langley Research Center. Previous work involving parallel stability computations of a boundary layer flow based on the conical flow approximation has shown that the measured onset of laminar-turbulent transition during the experiments can be correlated with the linear amplification of Tollmien- Schlichting (TS) and stationary crossflow (CF) instabilities in the swept wing boundary layer. Here, we examine the effects of the simplifying approximations in both basic state computation and the stability analysis, with the goal of quantifying the resulting changes in the N-factor correlations. Specifically, the basic states are computed by using full Navier-Stokes equations and the stability analysis is performed by using a nonorthogonal coordinate system that allows a clear distinction between planar TS and CF instabilities. Furthermore, the effects of curvature and nonparallel mean flow have been included in the stability computations based on the parabolized stability equations (PSE). The fully turbulent Reynolds-Averaged-Navier-Stokes (RANS) mean flow solutions show good agreement with the measured wall pressure distribution. Viscous-inviscid interactive effects are observed to be important because the shock fronts along the suction surface are influenced by the imposed transition front. The stability results confirm the previous findings related to TS amplification within the inboard region of the wing and the dominance of stationary CF modes in the outboard region. However, given the close proximity of the measured transition front and the dual shock system within the outer part of the wing, the onset of transition may well be shock limited within the outboard region. In general, the transition criterion based on the dual N-factor method with N TS = N CF = 6 is reasonably successful at correlating with the measured transition fronts at Re MAC = 15 million and AoA = 1.5, 2 degrees; however, the low values of the correlating N-factors at Re MAC = 17.5 million support the hypothesis that the measured transition at the higher Reynolds number may have been strongly influenced by the merging of turbulent wedges that originate from surface imperfections near the leading edge.

Boundary layer transition↗

NASA NTRS2020

TOI 564 b and TOI 905 b: Grazing and Fully Transiting Hot Jupiters Discovered by TESS

We report the discovery and confirmation of two new hot Jupiters discovered by the Transiting Exoplanet Survey Satellite(TESS): TOI 564 b and TOI 905 b. The transits of these two planets were initially observed by TESS with orbital periods of 1.651 and 3.739 days, respectively. We conducted follow-up observations of each system from the ground, including photometry in multiple filters, speckle interferometry, and radial velocity measurements. For TOI 564 b, our global fitting revealed a classical hot Jupiter with a mass of-+1.4630.0960.10MJand a radius of-+1.020.290.71RJ. Also a classical hot Jupiter, TOI 905 b has a mass of-+0.6670.0410.042MJand radius of-+1.1710.0510.053RJ. Both planets orbit Sun-like, moderately bright, mid-G dwarf stars with V11. While TOI 905 b fully transits its star, we found that TOI 564 b has a very high transit impact parameter of-+0.9940.0490.083, making it one of only∼20 known systems to exhibit a grazing transit and one of the brightest host stars among them. Therefore, TOI 564 b is one of the most attractive systems to search for additional nontransiting, smaller planets by exploiting the sensitivity of grazing transits to small changes in inclination and transit duration over a timescale of several years.

Exoplanet astronomy↗

NASA NTRS2021

Hypersonic Boundary-Layer Transition on Blunted Cones at Angle of Attack

Experimental studies of cones at several high-speed facilities have demonstrated that, for small nosetip bluntness, transition onset over a circular cone moves upstream along the leeward side and downstream along the windward side, but this trend may be reversed at large bluntness values, where transition onset moves downstream along the leeward side and upstream along the windward side. A theoretical and numerical investigation is performed to characterize the effects of nose bluntness on disturbance amplification over the circular cone for several angles of attack, with the goal of understanding the potential physical mechanisms behind the experimental observations. The three-dimensional laminar basic states over a 1.5 m long, 7-degree half-angle cone with 9.525 mm nosetip radius are computed for selected angles of attack values and freestream conditions that are selected to match the Mach 10 experiments conducted within the Hypervelocity Wind Tunnel 9 at the Arnold Engineering Development Complex (AEDC). The solutions at a freestream unit Reynolds number of 17.1 million per meter are used to perform detailed instability analyses for angles of attack equal to 0, 1, 3, and 5 degrees. Results indicate that the linear amplification of stationary crossflow waves along inflection lines may begin to influence transition along the acreage of the cone for angles of attack equal to or larger than 5 degrees. The measured trend in transition front with respect to increasing angle of attack is found to be consistent with the predicted increase in the amplification factors for Mack mode disturbances along the streamline trajectories. The increase in Mack mode amplification along the windward ray for higher angles of attack is shown to be the result of a progressively earlier entropy-layer swallowing. Computations also indicate that the transition amplification factor along the windward ray is not constant and increases with the angle of attack and that the transition #-factors along the leeward ray are rather small. The nonmodal analysis for zero degrees angle of attack shows that entropy-layer disturbances with appreciably strong energy growth can coexist with Mack mode instabilities at the measured transition location.

boundary layer transition↗

NASA NTRSDate not supplied

Transition Modeling Based on the Dual N-factor Method for the CRM-NLF Wind Tunnel Configuration

The dual N-factor method is used to model the boundary-layer transition over the common research model with natural laminar flow (CRM-NLF) aircraft configuration. The flow conditions match selected test conditions from a wind tunnel experiment in the National Transonic Facility at the NASA Langley Research Center. The paper presents a systematic methodology for transition prediction in the presence of a dual shock system and extends the prior capability for iteratively coupled computational fluid dynamics (CFD) predictions to incorporate three-dimensional, transonic wings. The method employs stability computations based on the linear parabolized stability equations (PSE), along with a dual N-factor criterion. The iterative process begins with the fully turbulent Reynolds-averaged-Navier-Stokes (RANS) mean flow solution. For the first iteration, a mean flow solution is calculated with an imposed transition front that aligns with the shock front from the fully turbulent solution. Subsequently, stability computations are performed along a set of streamlines across the wing to calculate the amplification of planar Tollmien-Schlichting (TS) and stationary crossflow (CF) modes. The transition criterion based on the dual N-factor method is used to infer the updated transition front and the process is successively repeated until convergence of the solution. Within three iterations, the predicted fronts for angles of attack of 1.45, 1.98, 2.46 and 2.94 degrees and a mean-aerodynamic-chord Reynolds number equal to 15 million, approach visual convergence in most regions of the studied cases, and the resulting predictions are in good agreement with the transition fronts deduced from measurements of temperature-sensitive paint. Even though surface pressure measurements based on fully-turbulent flow agree well with the measured pressure coefficient distributions, strong viscous-inviscid interaction effects cause significant shifts in the shock locations based on the imposed transition front, underscoring the intrusive nature of static pressure measurements using surface mounted ports on the CRM-NLF configuration.

Boundary Layer Transition↗

NASA NTRSDate not supplied

Transition Analysis for the Pazy Wing

The Pazy wing, designed as a benchmark for highly flexible wings that experience large deformations, presents intriguing nonlinear phenomena due to its unique geometry with spanwise varying static deformation and low Reynolds number flow conditions. These phenomena include limit cycle oscillation related to laminar separation bubbles, boundary-layer transition, and dynamic stall. The primary focus of this study is to investigate transition behavior on the sagged Pazy wing under static loading by using the shear-stress-transport (SST)-based Langtry-Menter 𝜸 − 𝑹𝒆𝜽𝒕 transition model in the NASA OVERFLOW and FUN3D solvers. Based on the steady-state results obtained via different variants of the Langtry-Menter model, we investigate the likely transition behavior over a range of incidence angles. The predicted flowfield on the sagged Pazy wing is strongly three dimensional and the application of turbulence index as a viable indicator of the transition front in such flows is also explored. The study demonstrates the limitations of the Langtry-Menter model when applied to low Reynolds number flows. We introduce a spanwise periodic configuration to simulate a narrow-span section of the Pazy wing, specifically centered on one of the 14 nearly equidistant ribs spanning the wing. The computational results demonstrate that the spanwise periodic configuration provides a straightforward environment for studying transition characteristics as well as demonstrating systematic grid convergence and successful code-to-code comparisons. The research offers useful insights into the transition characteristics of flexible wings under various loading conditions, contributing to the field of aeroelastic simulations.

CFD Modeling↗

NASA NTRSDate not supplied

Grid Refinement Techniques for the 𝜸-Re𝜽𝒕 Transition Model in FUN3D

There has been an increased focus on the overall accuracy and grid convergence of Reynolds-averaged Navier-Stokes (RANS)-based transition models from the recent AIAA and NATO-AVT workshops. Even though satisfactory grid convergence could be achieved for simple two-dimensional flow configurations, it required mesh counts that are substantially larger than those used in typical applications. In this paper, we focus our efforts on understanding how the grid resolution and topology influences the accuracy and convergence of results by studying the Schubauer and Skramstad flat-plate configuration and the NLF-0416 airfoil at an angle of attack equal to five degrees using FUN3D, a second-order finite-volume code. By focusing on these cases, we can analyze both natural and separation-induced transition scenarios. Multiple grid refinement strategies are investigated. First, we determine the relative effectiveness of zonal streamwise refinement in the transition region within structured grids as an alternative to the costly option of globally uniform refinement of a baseline grid. We also complement this zonal technique by globally varying the wall-normal resolution keeping the streamwise resolution fixed. The zonal streamwise refinement can accurately model natural transition in a flat-plate boundary layer and separation-induced transition, but struggles to accurately model natural transition in airfoil flows. A series of unstructured prismatic grids that have similar node counts and viscous wall spacings as the structured hexahedral grids are also tested, and they do not achieve grid convergence until an extremely fine resolution. Last, we employ adjoint-based unstructured grid adaptation in FUN3D to natural and separation-induced transition on the NLF-0416 airfoil. The adjoint-based refinement process converges to the same solution as the baseline family of structured grids, but leads to smaller errors on coarser grids.

Grid Adaptation↗

NASA NTRSDate not supplied

Modeling Boundary-Layer Transition in Subsonic Flow over a Swept Wing

Predicting the onset of boundary-layer transition is often more accurate using physics-based models that directly compute disturbance growth rather than phenomenological models often implemented into industrial CFD codes. The aim of this ongoing study is to calibrate linear, physics-based computations of transition in subsonic flows over swept wings against a large set of experimental data. Advancing the calibration of linear models of transition contributes to the CFD-Vision-2030 goal of automated boundary-layer transition prediction. This progress report uses the dual N-factor method to model transition over the swept NACA 64-2-015A wing. The flow conditions match selected test conditions from an extensive experimental dataset acquired from the NASA Ames 12-ft Pressure Tunnel. The OVERFLOW 2.4b flow solver is used to obtain laminar basic states based on an infinite-span assumption. Stability analyses are performed on 365 distinct configurations with linear stability theory (LST) and parabolized stability equations (PSE) from the Langley Stability and Transition Analysis Codes (LASTRAC), modeling the growth of Tollmien-Schlichting (TS) and stationary crossflow (SCF) disturbances. From a total of 67 data points for unswept, i.e., TS-dominant configurations, the critical N-factor based on PSE is found to be N_TS = 9. The SCF critical N-factor is found to be near 8 for the highly swept, SCF-dominant configurations. Dual N-factor curves for both LST and PSE computations demonstrate a high level of interaction between TS and SCF. It may be worthwhile to investigate an alternate metric to visualize maximal SCF amplification upstream of the transition location to account for the growth of SCF modes near the leading edge, which is not considered in the conventional applications of the dual N-factor criterion.

boundary-layer transition↗

NASA NTRSDate not supplied

Grid Refinement Techniques for the 𝜸-Re 𝜽 𝒕 Transition Model in FUN3D

There has been an increased focus on the overall accuracy and grid convergence of Reynolds-averaged Navier-Stokes (RANS)-based transition models from the recent AIAA and NATO-AVT workshops. Even though satisfactory grid convergence could be achieved for simple two-dimensional flow configurations, it required mesh counts that are substantially larger than those used in typical applications. In this paper, we focus our efforts on understanding how the grid resolution and topology influences the accuracy and convergence of results by studying the Schubauer and Skramstad flat-plate configuration and the NLF-0416 airfoil at an angle of attack equal to five degrees using FUN3D, a second-order finite-volume code. By focusing on these cases, we can analyze both natural and separation-induced transition scenarios. Multiple grid refinement strategies are investigated. First, we determine the relative effectiveness of zonal streamwise refinement in the transition region within structured grids as an alternative to the costly option of globally uniform refinement of a baseline grid. We also complement this zonal technique by globally varying the wall-normal resolution keeping the streamwise resolution fixed. The zonal streamwise refinement can accurately model natural transition in a flat-plate boundary layer and separation-induced transition, but struggles to accurately model natural transition in airfoil flows. A series of unstructured prismatic grids that have similar node counts and viscous wall spacings as the structured hexahedral grids are also tested, and they do not achieve grid convergence until an extremely fine resolution. Last, we employ adjoint-based unstructured grid adaptation in FUN3D to natural and separation-induced transition on the NLF-0416 airfoil. The adjoint-based refinement process converges to the same solution as the baseline family of structured grids, but leads to smaller errors on coarser grids.

Grid Adaptation↗

NASA NTRSDate not supplied

Transition Analysis for the Pazy Wing

The Pazy wing, designed as a benchmark for highly flexible wings that experience large deformations, presents intriguing nonlinear phenomena due to its unique geometry with spanwise varying static deformation and low Reynolds number flow conditions. These phenomena include limit cycle oscillation related to laminar separation bubbles, boundary-layer transition, and dynamic stall. The primary focus of this study is to investigate transition behavior on the sagged Pazy wing under static loading by using the shear-stress-transport (SST)-based Langtry-Menter 𝜸 − 𝑹𝒆𝜽𝒕 transition model in the NASA OVERFLOW and FUN3D solvers. Based on the steady-state results obtained via different variants of the Langtry-Menter model, we investigate the likely transition behavior over a range of incidence angles. The predicted flowfield on the sagged Pazy wing is strongly three dimensional and the application of turbulence index as a viable indicator of the transition front in such flows is also explored. The study demonstrates the limitations of the Langtry-Menter model when applied to low Reynolds number flows. We introduce a spanwise periodic configuration to simulate a narrow-span section of the Pazy wing, specifically centered on one of the 14 nearly equidistant ribs spanning the wing. The computational results demonstrate that the spanwise periodic configuration provides a straightforward environment for studying transition characteristics as well as demonstrating systematic grid convergence and successful code-to-code comparisons. The research offers useful insights into the transition characteristics of flexible wings under various loading conditions, contributing to the field of aeroelastic simulations.

CFD Modeling↗

NASA NTRSDate not supplied

Modeling Boundary-Layer Transition in Subsonic Flow over a Swept Wing

Predicting the onset of boundary-layer transition is often more accurate using physics-based models that directly compute disturbance growth rather than phenomenological models often implemented into industrial CFD codes. The aim of this ongoing study is to calibrate linear, physics-based computations of transition in subsonic flows over swept wings against a large set of experimental data. Advancing the calibration of linear models of transition contributes to the CFD-Vision-2030 goal of automated boundary-layer transition prediction. This progress report uses the dual N-factor method to model transition over the swept NACA 64-2-015A wing. The flow conditions match selected test conditions from an extensive experimental dataset acquired from the NASA Ames 12-ft Pressure Tunnel. The OVERFLOW 2.4b flow solver is used to obtain laminar basic states based on an infinite-span assumption. Stability analyses are performed on 365 distinct configurations with linear stability theory (LST) and parabolized stability equations (PSE) from the Langley Stability and Transition Analysis Codes (LASTRAC), modeling the growth of Tollmien-Schlichting (TS) and stationary crossflow (SCF) disturbances. From a total of 67 data points for unswept, i.e., TS-dominant configurations, the critical N-factor based on PSE is found to be N_TS = 9. The SCF critical N-factor is found to be near 8 for the highly swept, SCF-dominant configurations. Dual N-factor curves for both LST and PSE computations demonstrate a high level of interaction between TS and SCF. It may be worthwhile to investigate an alternate metric to visualize maximal SCF amplification upstream of the transition location to account for the growth of SCF modes near the leading edge, which is not considered in the conventional applications of the dual N-factor criterion.

computational modeling↗

DOE OSTI2023

Study of Seamless Microgrid Transition Operation Using Grid-Forming Inverters

This paper investigates operational techniques to achieve seamless (smooth) microgrid (MG) transitions by dispatching a grid-forming (GFM) inverter. In traditional approaches, the GFM inverter must switch between grid-following (GFL) and GFM control modes during MG transition operation. Today's inverter technology allows GFM inverters to always operate in GFM control mode, so it is worth exploring how to use them to achieve smooth MG transition operation. This paper proposes three operational techniques: a traditional scheme of switching between GFL and GFM control; a new scheme of consistent GFM control and shifting the droop intercept up before islanding operation; and a new scheme of consistent GFM control and shifting the droop intercept up before synchronization operation. A full hardware setup is established to compare the three techniques and showcase their implementations in real-world applications. The results show that the third technique outperforms the others and exhibits the best transition performance because the GFM inverter maintains the same operating points during the transition operation. Therefore, we conclude that ensuring smooth MG transition operation requires that the GFM inverter(s) maintain the same operating points (v, f, P, Q, and phase angle) during the transition operation in addition to minimizes the point of common coupling power flow.

grid-forming↗

DOE OSTI2023

Delineating the Impact of Transition‐Metal Crossover on Solid‐Electrolyte Interphase Formation with Ion Mass Spectrometry

Abstract Lithium‐metal batteries (LMB) employing cobalt‐free layered‐oxide cathodes are a sustainable path forward to achieving high energy densities, but these cathodes exhibit substantial transition‐metal dissolution during high‐voltage cycling. While transition‐metal crossover is recognized to disrupt solid‐electrolyte interphase (SEI) formation on graphite anodes, experimental evidence is necessary to demonstrate this for lithium‐metal anodes. In this work, advanced high‐resolution 3D chemical analysis is conducted with time‐of‐flight secondary‐ion mass spectrometry (TOF‐SIMS) to establish spatial correlations between the transition metals and electrolyte decomposition products found on cycled lithium‐metal anodes. Insights into the localization of various chemistries linked to crucial processes that define LMB performance, such as lithium deposition, SEI growth, and transition‐metal deposition are deduced from a precise elemental and spatial analysis of the SEI. Heterogenous transition‐metal deposition is found to perpetuate both heterogeneous SEI growth and lithium deposition on lithium‐metal anodes. These correlations are confirmed across various lithium‐metal anodes that are cycled with different cobalt‐free cathodes and electrolytes. An advanced electrolyte that is stable to higher voltages is shown to minimize transition‐metal crossover and its effects on lithium‐metal anodes. Overall, these results highlight the importance of maintaining uniform SEI coverage on lithium‐metal anodes, which is disrupted by transition‐metal crossover during operation at high voltages.

Chemistry↗

DOE OSTI2022

Disorder Dynamics in Battery Nanoparticles During Phase Transitions Revealed by Operando Single-Particle Diffraction

Structural and ion-ordering phase transitions limit the viability of sodium-ion intercalation materials in grid scale battery storage by reducing their lifetime. However, the combination of phenomena in nanoparticulate electrodes creates complex behavior that is difficult to investigate, especially on the single-nanoparticle scale under operating conditions. In this work, operando single-particle X-ray diffraction (oSP-XRD) is used to observe single-particle rotation, interlayer spacing, and layer misorientation in a functional sodium-ion battery. oSP-XRD is applied to Na 2/3 [Ni 1/3 Mn 2/3 ]O 2 , an archetypal P2-type sodium-ion-positive electrode material with the notorious P2-O2 phase transition induced by sodium (de)intercalation. Here, it is found that during sodium extraction, the misorientation of crystalline layers inside individual particles increases before the layers suddenly align just prior to the P2-O2 transition. The increase in the long-range order coincides with an additional voltage plateau signifying a phase transition prior to the P2-O2 transition. To explain the layer alignment, a model for the phase evolution is proposed that includes a transition from localized to correlated Jahn-Teller distortions. The model is anticipated to guide further characterization and engineering of sodium-ion intercalation materials with P2-O2 type transitions. oSP-XRD, therefore, opens a powerful avenue for revealing complex phase behavior in heterogeneous nanoparticulate systems.

25 ENERGY STORAGE↗