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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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At least 433 records · Page 24

Single Entity Electrochemistry in Nanopore Electrode Arrays: Ion Transport Meets Electron Transfer in Confined Geometries

Electrochemical measurements conducted in confined volumes provide a powerful and direct means to address scientific questions at the nexus of nanoscience, biotechnology, and chemical analysis. How are electron transfer and ion transport coupled in confined volumes and how does understanding them require moving beyond macroscopic theories? Also, how do these coupled processes impact electrochemical detection and processing? We address these questions by studying a special type of confined-volume architecture, the nanopore electrode array, or NEA, which is designed to be commensurate in size with physical scaling lengths, such as the Debye length, a concordance that offers performance characteristics not available in larger scale structures. The experiments described here depend critically on carefully constructed nanoscale architectures that can usefully control molecular transport and electrochemical reactivity. We begin by considering the experimental constraints that guide the design and fabrication of zero-dimensional nanopore arrays with multiple embedded electrodes. These zero-dimensional structures are nearly ideal for exploring how permselectivity and unscreened ion migration can be combined to amplify signals and improve selectivity by enabling highly efficient redox cycling. Our studies also highlight the benefits of arrays, in that molecules escaping from a single nanopore are efficiently captured by neighboring pores and returned to the population of active redox species being measured, benefits that arise from coupling ion accumulation and migration. These tools for manipulating redox species are well-positioned to explore single molecule and single particle electron transfer events through spectroelectrochemistry, studies which are enabled by the electrochemical zero-mode waveguide (ZMW), a special hybrid nanophotonic/nanoelectronic architecture in which the lower ring electrode of an NEA nanopore functions both as a working electrode to initiate electron transfer reactions and as the optical cladding layer of a ZMW. Furthermore, while the work described here is largely exploratory and fundamental, we believe that the development of NEAs will enable important applications that emerge directly from the unique coupled transport and electron-transfer capabilities of NEAs, including in situ molecular separation and detection with external stimuli, redox-based electrochemical rectification in individually encapsulated nanopores, and coupled sorters and analyzers for nanoparticles.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Accelerating Quantum Materials Development with Advances in Transmission Electron Microscopy

Quantum materials are driving a technology revolution in sensing, communication, and computing, while simultaneously testing many core theories of the past century. Materials such as topological insulators, complex oxides, superconductors, quantum dots, color center-hosting semiconductors, and other types of strongly correlated materials can exhibit exotic properties such as edge conductivity, multiferroicity, magnetoresistance, superconductivity, single photon emission, and optical-spin locking. These emergent properties arise and depend strongly on the material’s detailed atomic-scale structure, including atomic defects, dopants, and lattice stacking. In this review, we describe how progress in the field of electron microscopy (EM), including in situ and in operando EM, can accelerate advances in quantum materials and quantum excitations. We begin by describing fundamental EM principles and operation modes. We then discuss various EM methods such as (i) EM spectroscopies, including electron energy loss spectroscopy (EELS), cathodoluminescence (CL), and electron energy gain spectroscopy (EEGS); (ii) four-dimensional scanning transmission electron microscopy (4D-STEM); (iii) dynamic and ultrafast EM (UEM); (iv) complementary ultrafast spectroscopies (UED, XFEL); and (v) atomic electron tomography (AET). We describe how these methods could inform structure–function relations in quantum materials down to the picometer scale and femtosecond time resolution, and how they enable precision positioning of atomic defects and high-resolution manipulation of quantum materials. For each method, we also describe existing limitations to solve open quantum mechanical questions, and how they might be addressed to accelerate progress. Among numerous notable results, our review highlights how EM is enabling identification of the 3D structure of quantum defects; measuring reversible and metastable dynamics of quantum excitations; mapping exciton states and single photon emission; measuring nanoscale thermal transport and coupled excitation dynamics; and measuring the internal electric field and charge density distribution of quantum heterointerfaces- all at the quantum materials’ intrinsic atomic and near atomic-length scale. Finally, we conclude by describing open challenges for the future, including achieving stable sample holders for ultralow temperature (below 10K) atomic-scale spatial resolution, stable spectrometers that enable meV energy resolution, and high-resolution, dynamic mapping of magnetic and spin fields. With atomic manipulation and ultrafast characterization enabled by EM, quantum materials will be poised to integrate into many of the sustainable and energy-efficient technologies needed for the 21st century.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Magnet-superconductor hybrid quantum systems: a materials platform for topological superconductivity

Magnet–superconductor hybrid (MSH) systems have recently emerged as one of the most significant developments in condensed matter physics. This has generated, in the last decade, a steadily rising interest in the understanding of their unique properties. They have been proposed as one of the most promising platforms for the establishment of topological superconductivity, which holds high potential for application in future quantum information technologies. Their emergent electronic properties stem from the exchange interaction between the magnetic moments and the superconducting condensate. Given the atomic-level origin of such interaction, it is of paramount importance to investigate new magnet–superconductor hybrids at the atomic scale. In this regard, scanning tunneling microscopy (STM) and spectroscopy are playing a crucial role in the race to unveil the fundamental origin of the unique properties of MSH systems, with the aim to discover new hybrid quantum materials capable of hosting topologically non-trivial unconventional superconducting phases. In particular, the combination of STM studies with tight-binding model calculations have represented, so far, the most successful approach to unveil and explain the emergent electronic properties of MSHs. The scope of this review is to offer a broad perspective on the field of MSHs from an atomic-level investigation point-of-view. The focus is on discussing the link between the magnetic ground state hosted by the hybrid system and the corresponding emergent superconducting phase. This is done for MSHs with both one-dimensional (atomic chains) and two-dimensional (atomic lattices and thin films) magnetic systems proximitized to conventional s-wave superconductors. We present a systematic categorization of the experimentally investigated systems with respect to defined experimentally accessible criteria to verify or falsify the presence of topological superconductivity and Majorana edge modes. The discussion will start with an introduction to the physics of Yu–Shiba–Rusinov bound states at magnetic impurities on superconducting surfaces. This will be used as a base for the discussion of magnetic atomic chains on superconductors, distinguishing between ferromagnetic, antiferromagnetic and non-collinear magnetic ground states. A similar approach will be used for the discussion of magnetic thin film islands on superconductors. Given the vast number of publications on the topic, we limit ourselves to discuss works which are most relevant to the search for topological superconductivity.

Majorana states↗

Predicting resistive wall mode stability in NSTX through balanced random forests and counterfactual explanations

Abstract Recent progress in the disruption event characterization and forecasting framework has shown that machine learning guided by physics theory can be easily implemented as a supporting tool for fast computations of ideal stability properties of spherical tokamak plasmas. In order to extend that idea, a customized random forest (RF) classifier that takes into account imbalances in the training data is hereby employed to predict resistive wall mode (RWM) stability for a set of high beta discharges from the NSTX spherical tokamak. More specifically, with this approach each tree in the forest is trained on samples that are balanced via a user-defined over/under-sampler. The proposed approach outperforms classical cost-sensitive methods for the problem at hand, in particular when used in conjunction with a random under-sampler, while also resulting in a threefold reduction in the training time. In order to further understand the model’s decisions, a diverse set of counterfactual explanations based on determinantal point processes (DPP) is generated and evaluated. Via the use of DPP, the underlying RF model infers that the presence of hypothetical magnetohydrodynamic activity would have prevented the RWM from concurrently going unstable, which is a counterfactual that is indeed expected by prior physics knowledge. Given that this result emerges from the data-driven RF classifier and the use of counterfactuals without hand-crafted embedding of prior physics intuition, it motivates the usage of counterfactuals to simulate real-time control by generating the β N levels that would have kept the RWM stable for a set of unstable discharges.

70 PLASMA PHYSICS AND FUSION TECHNOLOGY↗

Effects of strain, disorder, and Coulomb screening on free-carrier mobility in doped cadmium oxide

Here, the interplay of stress, disorder, and Coulomb screening dictating the mobility of doped cadmium oxide (CdO) is examined using Raman spectroscopy to identify the mechanisms driving dopant incorporation and scattering within this emerging infrared optical material. Specifically, multi-wavelength Raman and UV-vis spectroscopies are combined with electrical Hall measurements on a series of yttrium (X = Y) and indium (X = In) doped X:CdO thin-films. Hall measurements confirm n-type doping and establish carrier concentrations and mobilities. Spectral fitting along the low-frequency Raman combination bands, especially the TA+TO(X) mode, reveals that the evolution of strain and disorder within the lattice as a function of dopant concentration is strongly correlated with mobility. Coupling between the electronic and lattice environments was examined through analysis of first- and second-order longitudinal–optical phonon–plasmon coupled modes that monotonically decrease in energy and asymmetrically broaden with increasing dopant concentration. By fitting these trends to an impurity-induced Fröhlich model for the Raman scattering intensity, exciton–phonon and exciton–impurity coupling factors are quantified. These coupling factors indicate a continual decrease in the amount of ionized impurity scattering with increasing dopant concentration and are not as well correlated with mobility. This shows that lattice strain and disorder are the primary determining factors for mobility in donor-doped CdO. In aggregate, the study confirms previously postulated defect equilibrium arguments for dopant incorporation in CdO while at the same time identifying paths for its further refinement.

42 ENGINEERING↗

FEBIP for functional nanolithography of 2D nanomaterials

Lithographic patterning on emerging nanomaterials is one of essential ingredients for the development of new functional nanomaterial and device systems. Focused electron beam induced processing (FEBIP) in combination with an on-demand reconfigurable precursor injection system enables the highest resolution and controllability of nanolithography on two-dimensional (2D) nanomaterials. FEBIP allows for localized atomic-to-nanoscale engineering of nanomaterials and devices in a multi-mode format including geometrical patterning, functionalization/defect formation/doping, metal/metal oxide deposition, interface fusion and activation, active channel cleaning. This chapter discusses the scientific bases and showcases the state-of-the-art FEBIP technologies with a specific focus on functional lithography of 2D nanomaterials and provides future prospects of FEBIP technologies to address real industrial needs for the development of high-performance, next-generation functional devices.

2D materials, nanolithography, focused electron be↗

Epitaxial stabilization of thin films of the frustrated Ge-based spinels

Frustrated magnets can host numerous exotic many-body quantum and topological phenomena. GeNi 2 O 4 is a three-dimensional S=1 frustrated magnet with an unusual two-stage transition to the two-dimensional antiferromagnetic ground state, while GeCu 2 O 4 is a high-pressure phase with a strongly tetragonally elongated spinel structure and magnetic lattice formed by S=1/2 CuO 2 linear chains with frustrated interchain exchange interactions and exotic magnetic behavior. Here, we report on the thin-film epitaxial stabilization of these two compounds. The developed growth mode, surface morphology, crystal structure, and copper valence state were characterized by in situ reflection high-energy electron diffraction, atomic force microscopy, x-ray reflectivity, x-ray diffraction, x-ray photoelectron spectroscopy, and resonant x-ray absorption spectroscopy. Our results pave an alternative route to the comprehensive investigation of the puzzling magnetic properties of these compounds and the exploration of emergent features driven by strain.

36 MATERIALS SCIENCE↗

Constructing protein polyhedra via orthogonal chemical interactions

Many proteins exist naturally as symmetrical homooligomers or homopolymers. The emergent structural and functional properties of such protein assemblies have inspired extensive efforts in biomolecular design2–5. As synthesized by ribosomes, proteins are inherently asymmetric. Therefore, they must acquire multiple surface patches that selectively associate to generate the different symmetry elements needed to form higher-order architectures—a daunting task for protein design. Here we address this problem using an inorganic chemical approach, whereby multiple modes of protein–protein interactions and symmetry are simultaneously achieved by selective, ‘one-pot’ coordination of soft and hard metal ions. We show that a monomeric protein (protomer) appropriately modified with biologically inspired hydroxamate groups and zinc-binding motifs assembles through concurrent Fe 3+ and Zn 2+ coordination into discrete dodecameric and hexameric cages. Our cages closely resemble natural polyhedral protein architectures and are, to our knowledge, unique among designed systems in that they possess tightly packed shells devoid of large apertures. At the same time, they can assemble and disassemble in response to diverse stimuli, owing to their heterobimetallic construction on minimal interprotein-bonding footprints. With stoichiometries ranging from [2 Fe:9 Zn:6 protomers] to [8 Fe:21 Zn:12 protomers], these protein cages represent some of the compositionally most complex protein assemblies—or inorganic coordination complexes—obtained by design.

36 MATERIALS SCIENCE↗

Sustainable Public Transport: Providing Responsive, On-Demand Service with Clean Energy

The National Renewable Energy Laboratory (NREL) uses the Mobility Energy Productivity (MEP) as a metric and a lens to guide applied research into high performance public mobility. In the current initiative to abate global warming, the US needs not only zero-emission vehicles in the transit fleet (such as buses and shuttles) but also time- and cost-effective services to connect people with goods, services and employment toward a high-quality of life. Our current transportation system is overly dependent on personally-owned automobiles for high quality mobility, with public modes being less viable in many areas. Simply electrifying the drivetrains of existing public transit modes will fail to improve the quality of mobility for those that do not have access to private automobiles. The slow rebound by transit from the pandemic reveals the need to reinvent public transit service. Using the MEP lens, NREL researchers have tracked various novel developments in the public mobility space, with the confluence of shared, on-demand transit (ODT) services using light duty vehicles emerging as a key enabler of high-efficiency public mobility. Deployments such as those in Arlington, TX, Dallas, TX, Fort Erie, ON, and Innisfil, ON showcase the use of fleets of light-duty vehicles as the basis for community circulation and first/last mile to intra-regional transit. ODT services have demonstrated improvements in being more time efficient for riders, more energy efficient in operation (even before the introduction of fully electric vehicles), as well as being cost effective. It appears that aspects of the long-awaited promise of Personal Rapid Transit from the 1970s are beginning to be realized through ODT deployments, leveraging transportation network company (TNC) logistics, popularized by Uber and Lyft, but applied to public mobility. Currently, manually driven ODT operations are already cost competitive with traditional transit systems on a cost per ride basis, and full automation promises to reduce costs by 50% while providing additional safety and verified customer service. Connecting these ODT systems with efficient and effective intra-regional backbone transit service is the next step, with transit agencies like DART providing early results. This discussion will walk through the evidence for this postulated outcome and show results from a series of case-studies.

ADVANCED PROPULSION SYSTEMS,ENERGY PLANNING, POLIC↗

Orbital inversion and emergent lattice dynamics in infinite layer CaCoO 2

The layered cobaltate CaCoO 2 exhibits a unique herringbone-like structure. Serving as a potential prototype for a new class of complex lattice patterns, we study the properties of CaCoO 2 using X-ray absorption spectroscopy (XAS) and resonant inelastic X-ray scattering (RIXS). Our results reveal a significant inter-plane hybridization between the Ca 4s- and Co 3d- orbitals, leading to an inversion of the textbook orbital occupation of a square planar geometry. Further, our RIXS data reveal a strong low energy mode, with anomalous intensity modulations as a function of momentum transfer close to a quasi-static response. These findings indicate that the newly discovered herringbone structure exhibited in CaCoO 2 may serve as a promising laboratory for the design of materials having strong electronic, orbital and lattice correlations.

Electronic properties and materials↗

Optical Durability of Contemporary PV Encapsulants Through Artificial UV Weathering

Modern c-Si photovoltaic (PV) cells provide high performance but can be vulnerable to ultraviolet light induced degradation (UV-ID). Encapsulants, if chosen correctly, can mitigate UV-ID of the PV cell. Here, we explore performance and durability of 14 commercial encapsulant materials before, during, and after irradiation with UV-containing light. Materials include contemporary, polymer-based encapsulants with a base polymer of poly (ethylene co-vinyl acetate) (EVA), polyethylene-..alpha..-olefin (POE), or their composite (EPE). Polymers contain additives that induce UV-blocking, UV-transmitting, or UV-downshifting properties. We use test coupons to study degradation in a chamber held at 65 degrees C under a xenon light source for up to 4000 h of exposure, corresponding to a cumulative dose of 11.5 MJ/m2 at 340 nm. We examine optical properties including spectral transmittance, yellowness index and spectral fluorescence, considering changes to both the encapsulant and glass as a function of weathering time. Degradation modes identified include discoloration, changes to UV cutoff wavelength, changes to solar-weighted transmittance, and most notably a change to the UV-managing properties of some additives. We propose the use of solar-weighted transmittance in the 300- to 400-nm range to better track performance changes in the UV region associated with the UV-related additive. This is especially relevant for the emerging class of UV-downshifting additives, as metrics like UV-cutoff can understate the degree of degradation or change in these materials. While most encapsulants show very little change after weathering, some show significant changes that directly impact how much UV light would reach an underlying cell.

14 SOLAR ENERGY↗

Terahertz electric-field-driven dynamical multiferroicity in SrTiO 3

The emergence of collective order in matter is among the most fundamental and intriguing phenomena in physics. In recent years, the dynamical control and creation of novel ordered states of matter not accessible in thermodynamic equilibrium is receiving much attention. The theoretical concept of dynamical multiferroicity has been introduced to describe the emergence of magnetization due to time-dependent electric polarization in non-ferromagnetic materials. In simple terms, the coherent rotating motion of the ions in a crystal induces a magnetic moment along the axis of rotation. Here we provide experimental evidence of room-temperature magnetization in the archetypal paraelectric perovskite SrTiO 3 due to this mechanism. We resonantly drive the infrared-active soft phonon mode with an intense circularly polarized terahertz electric field and detect the time-resolved magneto-optical Kerr effect. A simple model, which includes two coupled nonlinear oscillators whose forces and couplings are derived with ab initio calculations using self-consistent phonon theory at a finite temperature, reproduces qualitatively our experimental observations. A quantitatively correct magnitude was obtained for the effect by also considering the phonon analogue of the reciprocal of the Einstein–de Haas effect, which is also called the Barnett effect, in which the total angular momentum from the phonon order is transferred to the electronic one. Our findings show a new path for the control of magnetism, for example, for ultrafast magnetic switches, by coherently controlling the lattice vibrations with light.

36 MATERIALS SCIENCE↗

Combinatorial split-ring and spiral metaresonator for efficient magnon-photon coupling

Developing hybrid materials and structures for electromagnetic wave engineering has been a promising route towards novel functionalities and tunabilities in many modern applications. Despite its established success in engineering optical light and terahertz waves, the implementation of metaresonators operating in the microwave band is still emerging, especially the implementation of metaresonators that allow on-chip integration and size miniaturization, which is crucial for developing hybrid quantum systems in the microwave band. In this work, we present a microwave metaresonator consisting of split-ring and spiral resonators, and implement it for the investigation of photon-magnon coupling for hybrid magnonic applications. We observe broadened bandwidth of the split-ring modes augmented by the additional spiral resonator, and, by coupling the modes to a magnetic sample, the resultant photon-magnon coupling can be significantly enhanced by more than tenfold. Furthermore, our work suggests that combinatorial, hybrid microwave resonators may be a promising approach towards future development and implementation of photon-magnon coupling in hybrid magnonic systems.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗

Regioselective On-Surface Synthesis of [3]Triangulene Graphene Nanoribbons

The integration of low-energy states into bottom-up engineered graphene nanoribbons (GNRs) is a robust strategy for realizing materials with tailored electronic band structure for nanoelectronics. Low-energy zero-modes (ZMs) can be introduced into nanographenes (NGs) by creating an imbalance between the two sublattices of graphene. This phenomenon is exemplified by the family of [n]triangulenes (n ϵ $\mathbb{N}$). Here, we demonstrate the synthesis of [3]triangulene-GNRs, a regioregular one-dimensional (1D) chain of [3]triangulenes linked by five-membered rings. Hybridization between ZMs on adjacent [3]triangulenes leads to the emergence of a narrow band gap, E g,exp ~ 0.7 eV, and topological end states that are experimentally verified using scanning tunneling spectroscopy. Tight-binding and first-principles density functional theory calculations within the local density approximation corroborate our experimental observations. Our synthetic design takes advantage of a selective on-surface head-to-tail coupling of monomer building blocks enabling the regioselective synthesis of [3]triangulene-GNRs. Detailed ab initio theory provides insights into the mechanism of on-surface radical polymerization, revealing the pivotal role of Au-C bond formation/breakage in driving selectivity.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Green microalga Chromochloris zofingiensis conserves substrate uptake pattern but changes their metabolic uses across trophic transition

The terrestrial green alga Chromochloris zofingiensis is an emerging model species with potential applications including production of triacylglycerol or astaxanthin. How C. zofingiensis interacts with the diverse substrates during trophic transitions is unknown. To characterize its substrate utilization and secretion dynamics, we cultivated the alga in a soil-based defined medium in transition between conditions with and without glucose supplementation. Then, we examined its exometabolite and endometabolite profiles. This analysis revealed that regardless of trophic modes, C. zofingiensis preferentially uptakes exogenous lysine, arginine, and purines, while secreting orotic acid. Here, we obtained metabolomic evidences that C. zofingiensis may use arginine for putrescine synthesis when in transition to heterotrophy, and for the TCA cycle during transition to photoautotrophy. We also report that glucose and fructose most effectively inhibited photosynthesis among thirteen different sugars. The utilized or secreted metabolites identified in this study provide important information to improve C. zofingiensis cultivation, and to expand its potential industrial and pharmaceutical applications.

59 BASIC BIOLOGICAL SCIENCES↗

A comparison between residential relocation timing of Sydney and Chicago residents: A Bayesian survival analysis

We report that understanding households' behaviour in residential relocation timing is of great importance in the field of transport engineering and economics. This research aims to develop a residential relocation model by considering the potential dynamic impacts of other households' decisions and variables, including economic and demographic attributes, housing features, intra-household decision-making structures, travel mode choice, and other life-course attributes. A multivariate parametric survival model with both fixed and time-varying covariates is developed. To the best of the authors' knowledge, this study is the first paper in the literature of residential relocation timing to propose the use of a Bayesian model in contrast to the widely used classic frequentist approach and have conducted a discussion on its advantages. An emerging residential relocation dataset collected for two cities in Australia and the USA (Sydney and Chicago cities) has been used, which covers residence, vehicle ownership, occupation, education, economic and demographic attributes of respondents. A comprehensive comparison between the results of two cities and a comparison between two Bayesian and frequentist approaches are made. This study confirms the impact of life-course variables, intra-household decision-making behaviours, and sociodemographic attributes on home mobility. According to the model outputs, the accelerating or decelerating impact of explanatory variables on the relocation timing has been almost the same in the two cities. The Bayesian model was confirmed to have some advantages over the frequentist model, including being straightforward to interpret, availability of making inferences on the results, and ease of handling complex models, and optimisation convergence complexities.

99 GENERAL AND MISCELLANEOUS↗

Selective isomer emission via funneling of exciton polaritons

Polaritons in organic systems has shown the potential to modify chemical properties and to mediate long-range energy transfer between individual chromophores, among other capabilities. Here, we demonstrate that strong coupling and formation of organic exciton-polaritons can be used to selectively tune the isomer emission of organic molecules. By taking advantage of their delocalized and hybrid character, polaritons emerging in the strong coupling regime open a new relaxation pathway that allows for an efficient funneling of the excitation between the molecular isomers. We implement this by strong coupling to trans-DCS (E-4-dimethylamino-4'cyanostilbene)molecules, which present two isomers in different amounts when immersed in a polymer matrix. Thanks to this new relaxation pathway, the photoexcitation that is first shared by the common polaritonic mode is then selectively funneled to the excited states of one of the isomers, recognizing pure emission from the isomeric states that do not contribute to emission under normal conditions.

59 BASIC BIOLOGICAL SCIENCES↗

Enabling "Fuel" Switching through On-Demand Wind Control

This work demonstrates that classical shear-flow stability theory can be successfully applied to modify wind turbine wakes and also explains the success of several emerging, empirically-arrived control methods (i.e., dynamic induction and helix control). Linear stability theory predictions are extended to include the effects of non-axisymmetric inflow profiles, such as wind shear, which is shown to not strongly affect the primary forcing frequency. The predictions, as well as idealized large-eddy simulations using actuator-line representation of the turbine blades, agree that the n = 0 and ±1 modes have faster initial growth rates than higher-order modes, suggesting the lower-order modes are more appropriate for wake control. Exciting the lower-order modes with periodic pitching of the blades produces higher entrainment into the wake and consequently faster wake recovery.

17 WIND ENERGY↗