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At least 343 records · Page 19

Ferrielectricity in the Archetypal Antiferroelectric, PbZrO 3

Antiferroelectric materials, where the transition between antipolar and polar phase is controlled by external electric fields, offer exceptional energy storage capacity with high efficiencies, giant electrocaloric effect, and superb electromechanical response. PbZrO 3 is the first discovered and the archetypal antiferroelectric material. Nonetheless, substantial challenges in processing phase pure PbZrO 3 have limited studies of the undoped composition, hindering understanding of the phase transitions in this material or unraveling the controversial origins of a low-field ferroelectric phase observed in lead zirconate thin films. Here, leveraging highly oriented PbZrO 3 thin films, a room-temperature ferrielectric phase is observed in the absence of external electric fields, with modulations of amplitude and direction of the spontaneous polarization and large anisotropy for critical electric fields required for phase transition. The ferrielectric state observations are qualitatively consistent with theoretical predictions, and correlate with very high dielectric tunability, and ultrahigh strains (up to 1.1%). This work suggests a need for re-evaluation of the fundamental science of antiferroelectricity in this archetypal material.

36 MATERIALS SCIENCE↗

All‐Liquid Reconfigurable Electronics Using Jammed MXene Interfaces

Abstract Rigid, solid‐state components represent the current paradigm for electronic systems, but they lack post‐production reconfigurability and pose ever‐increasing challenges to efficient end‐of‐life recycling. Liquid electronics may overcome these limitations by offering flexible in‐the‐field redesign and separation at end‐of‐life via simple liquid phase chemistries. Up to now, preliminary work on liquid electronics has focused on liquid metal components, but these devices still require an encapsulating polymer and typically use alloys of rare elements like indium. Here, using the self‐assembly of jammed 2D titanium carbide (Ti 3 C 2 T x ) MXene nanoparticles at liquid–liquid interfaces, “all‐liquid” electrically conductive sheets, wires, and simple functional devices are described including electromechanical switches and photodetectors. These assemblies combine the high conductivity of MXene nanosheets with the controllable form and reconfigurability of structured liquids. Such configurations can have applications not only in electronics, but also in catalysis and microfluidics, especially in systems where the product and substrate have affinity for solvents of differing polarity.

36 MATERIALS SCIENCE↗

Defect‐Induced, Ferroelectric‐Like Switching and Adjustable Dielectric Tunability in Antiferroelectrics

Abstract Antiferroelectrics, which undergo a field‐induced phase transition to ferroelectric order that manifests as double‐hysteresis polarization switching, exhibit great potential for dielectric, electromechanical, and electrothermal applications. Compared to their ferroelectric cousins, however, considerably fewer efforts have been made to understand and control antiferroelectrics. Here, it is demonstrated that the polarization switching behavior of an antiferroelectric can be strongly influenced and effectively regulated by point defects. In films of the canonical antiferroelectric PbZrO 3 , decreasing oxygen pressure during deposition (and thus increasing adatom kinetic energy) causes unexpected “ferroelectric‐like” polarization switching although the films remain in the expected antiferroelectric orthorhombic phase. This “ferroelectric‐like” switching is correlated with the creation of bombardment‐induced point‐defect complexes which pin the antiferroelectric–ferroelectric phase boundaries, and thus effectively delay the phase transition under changing field. The effective pinning energy is extracted via temperature‐dependent switching‐kinetics studies. In turn, by controlling the concentration of defect complexes, the dielectric tunability of the PbZrO 3 can be adjusted, including being able to convert between “positive” and “negative” tunability near zero field. This work reveals the important role and strong capability of defects to engineer antiferroelectrics for new performance and functionalities.

Pan, Hao↗

Silicon-Lattice-Matched Boron-Doped Gallium Phosphide: A Scalable Acousto-Optic Platform

The compact size, scalability, and strongly confined fields in integrated photonic devices enable new functionalities in photonic networking and information processing, both classical and quantum. Gallium phosphide (GaP) is a promising material for active integrated photonics due to its high refractive index, wide bandgap, strong nonlinear properties, and large acousto-optic figure of merit. Here, this study demonstrates that silicon-lattice-matched boron-doped GaP (BGaP), grown at the 12-inch wafer scale, provides similar functionalities as GaP. BGaP optical resonators exhibit intrinsic quality factors exceeding 25,000 and 200,000 at visible and telecom wavelengths, respectively. It further demonstrates the electromechanical generation of low-loss acoustic waves and an integrated acousto-optic (AO) modulator. High-resolution spatial and compositional mapping, combined with ab initio calculations, indicate two candidates for the excess optical loss in the visible band: the silicon-GaP interface and boron dimers. These results demonstrate the promise of the BGaP material platform for the development of scalable AO technologies at telecom and provide potential pathways toward higher performance at shorter wavelengths.

36 MATERIALS SCIENCE↗

Highly Responsive Polar Vortices in All‐Ferroelectric Heterostructures

Abstract The discovery of polar vortices and skyrmions in ferroelectric‐dielectric superlattices [such as (PbTiO 3 ) n /(SrTiO 3 ) n ] has ushered in an era of novel dipolar topologies and corresponding emergent phenomena. The key to creating such emergent features has generally been considered to be related to counterpoising strongly polar and non‐polar materials thus creating the appropriate boundary conditions. This limits the utility these materials can have, however, by rendering (effectively) half of the structure unresponsive to applied stimuli. Here, using advanced thin‐film deposition and an array of characterization and simulation approaches, polar vortices are realized in all‐ferroelectric trilayers, multilayers, and superlattices built from the fundamental building block of (PbTiO 3 ) n /(Pb x Sr 1− x TiO 3 ) n wherein in‐plane ferroelectric polarization in the Pb x Sr 1− x TiO 3 provides the appropriate boundary conditions. These superlattices exhibit substantially enhanced electromechanical and ferroelectric responses in the out‐of‐plane direction that arise from the ability of the polarization in both layers to rotate to the out‐of‐plane direction under field. In the in‐plane direction, the layers are found to be strongly coupled during switching and when heterostructured with ferroelectric‐dielectric building blocks, it is possible to produce multistate switching. This approach expands the realm of systems supporting emergent dipolar texture formation and does so with entirely ferroelectric materials thus greatly improving their responses.

Kavle, Pravin↗

Mechanical Resonant Sensing of Spin Texture Dynamics in a 2D Antiferromagnet

Abstract The coupling between the spin degrees of freedom and macroscopic mechanical motions, including striction, shearing, and rotation, has attracted wide interest with applications in actuation, transduction, and information processing. Experiments so far have established the mechanical responses to the long‐range ordered or isolated single spin states. However, it remains elusive whether mechanical motions can couple to a different type of magnetic structure, the non‐collinear spin textures, which exhibit nanoscale spatial variations of spin (domain walls, skyrmions,etc.) and are promising candidates to realize high‐speed computing devices. Here, collective spin texture dynamics is detected with nanoelectromechanical resonators fabricated from 2D antiferromagnetic (AFM) MnPS 3 with 10 −9 strain sensitivity. By examining radio frequency mechanical oscillations under magnetic fields, new magnetic transitions are identified with sharp dips in resonant frequency. They are attributed to collective AFM domain wall motions as supported by the analytical modeling of magnetostriction and large‐scale spin‐dynamics simulations. Additionally, an abnormally large modulation in the mechanical nonlinearity at the transition field infers a fluid‐like response due to ultrafast domain motion. The work establishes a strong coupling between spin texture and mechanical dynamics, laying the foundation for electromechanical manipulation of spin texture and developing quantum hybrid devices.

Chemistry↗

Polarization Switching on the Open Surfaces of the Wurtzite Ferroelectric Nitrides: Ferroelectric Subsystems and Electrochemical Reactivity

Binary ferroelectric nitrides are promising materials for information technologies and power electronics. However, polarization switching in these materials is highly unusual. From the structural perspective, polarization reversal is associated with the change of the effective polarity at the surfaces and interfaces from N‐to‐M terminated, suggesting strong coupling between ferroelectric and chemical phenomena. Phenomenologically, macroscopic studies demonstrate the presence of complex time dependent phenomena including wake‐up. Here, in this study, the polarization switching using the multidimensional high‐resolution piezoresponse force microscopy (PFM) and spectroscopy is explored, detecting both the evolution of induced ferroelectric domain, electromechanical response, and surface deformation during first‐order reversal curve measurements. The presence of two weakly coupled ferroelectric subsystems are demonstrated and the bias‐induced electrochemical reactivity. The observed behaviors are very similar to the recent studies of other wurtzite system but additionally include electrochemical reactivity, suggesting the universality of these behaviors for the wurtzite binary ferroelectrics. These studies suggest potential of high‐resolution multimodal PFM spectroscopies to resolve complex coupled polarization dynamics in materials. Furthermore, these PFM based studies are fully consistent with the recent electron microscopy observations of the shark‐teeth like ferroelectric domains in nitrides. Hence, it is believed that these studies establish the universal phenomenological picture of polarization switching in binary wurtzite.

36 MATERIALS SCIENCE↗

Machine Learning Reveals Memory of the Parent Phases in Ferroelectric Relaxors Ba(Ti$_{1-x}$,Zr x )O 3

Machine learning has been establishing its potential in multiple areas of condensed matter physics and materials science. Here, in this work, an unsupervised machine learning workflow is developed and used within a framework of first-principles-based atomistic simulations to investigate phases, phase transitions, and their structural origins in ferroelectric relaxors, Ba(Ti 1-x ,Zr x )O 3 . The applicability of the workflow is first demonstrated to identify phases and phase transitions in the parent compound, a prototypical ferroelectric BaTiO 3 . Then the workflow is applied for Ba(Ti 1-x ,Zrx)O 3 with x ≤ 0.25 to reveal i) that some of the compounds bear a subtle memory of BaTiO 3 phases beyond the point of the pinched phase transition, which could contribute to their enhanced electromechanical response; ii) the existence of peculiar phases with delocalized precursors of nanodomains—likely candidates for the controversial polar nanoregions; and iii) nanodomain phases for the largest concentrations of x.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗

Optimizing Piezoelectric Nanocomposites by High‐Throughput Phase‐Field Simulation and Machine Learning

Abstract Piezoelectric nanocomposites with oxide fillers in a polymer matrix combine the merit of high piezoelectric response of the oxides and flexibility as well as biocompatibility of the polymers. Understanding the role of the choice of materials and the filler‐matrix architecture is critical to achieving desired functionality of a composite towards applications in flexible electronics and energy harvest devices. Herein, a high‐throughput phase‐field simulation is conducted to systematically reveal the influence of morphology and spatial orientation of an oxide filler on the piezoelectric, mechanical, and dielectric properties of the piezoelectric nanocomposites. It is discovered that with a constant filler volume fraction, a composite composed of vertical pillars exhibits superior piezoelectric response and electromechanical coupling coefficient as compared to the other geometric configurations. An analytical regression is established from a linear regression‐based machine learning model, which can be employed to predict the performance of nanocomposites filled with oxides with a given set of piezoelectric coefficient, dielectric permittivity, and stiffness. This work not only sheds light on the fundamental mechanism of piezoelectric nanocomposites, but also offers a promising material design strategy for developing high‐performance polymer/inorganic oxide composite‐based wearable electronics.

42 ENGINEERING↗

Thickness-Dependent Thermal Conductivity and Phonon Mean Free Path Distribution in Single-Crystalline Barium Titanate

Nanosized perovskite ferroelectrics are widely employed in several electromechanical, photonics, and thermoelectric applications. Scaling of ferroelectric materials entails a severe reduction in the lattice (phonon) thermal conductivity, particularly at sub-100 nm length scales. Such thermal conductivity reduction can be accurately predicted using the information of phonon mean free path (MFP) distribution. The current understanding of phonon MFP distribution in perovskite ferroelectrics is still inconclusive despite the critical thermal management implications. Here, high-quality single-crystalline barium titanate (BTO) thin films, a representative perovskite ferroelectric material, are grown at several thicknesses. Using experimental thermal conductivity measurements and first-principles based modeling (including four-phonon scattering), the phonon MFP distribution is determined in BTO. The simulation results agree with the measured thickness-dependent thermal conductivity. The results show that the phonons with sub-100 nm MFP dominate the thermal transport in BTO, and phonons with MFP exceeding 10 nm contribute ≈35% to the total thermal conductivity, in significant contrast to previously published experimental results. The experimentally validated phonon MFP distribution is consistent with the theoretical predictions of other complex crystals with strong anharmonicity. This work paves the way for thermal management in nanostructured and ferroelectric-domain-engineered systems for oxide perovskite-based functional materials.

36 MATERIALS SCIENCE↗

The Interplay Between Ferroelectricity and Electrochemical Reactivity on the Surface of Binary Ferroelectric Al x B 1–x N

Polarization dynamics and domain structure evolution in ferroelectric Al 0.93 B 0.07 N are studied using piezoresponse force microscopy and spectroscopies in ambient and controlled atmosphere environments. The application of negative unipolar and bipolar first-order reverse curve (FORC) waveforms leads to a protrusion-like feature on the Al 0.93 B 0.07 N surface and a reduction of electromechanical response due to electrochemical reactivity. A surface change is also observed on the application of fast alternating current bias. At the same time, the application of positive biases does not lead to surface changes. Comparatively in a controlled glove box atmosphere, stable polarization patterns can be observed, with minuscule changes in surface morphology. This surface morphology change is not isolated to applying biases to free surface, a similar topographical change is also observed at the electrode edges when cycling a capacitor in an ambient environment. The study suggests that surface electrochemical reactivity may have a significant impact on the functionality of this material in the ambient environment. However, even in the controlled atmosphere, the participation of the surface ions in polarization switching phenomena and ionic compensation is possible.

36 MATERIALS SCIENCE↗

In situ and operando force-based atomic force microscopy for probing local functionality in energy storage materials

Electrochemical energy storage is the key enabling component of electric vehicles and solar-/wind-based energy technologies. The enhancement of energy stored requires the detailed understanding of charge storage mechanisms and local electrochemical and electromechanical phenomena over a variety of length scales from atoms to full cells. Classical electrochemical techniques, such as voltammetry, represent the macroscopic electrochemical properties, and consequently do not allow to extract important information about local electrochemical reactions, ions adsorption, intercalations, and transport. Understanding, controlling, and tuning the local electrochemical functionalities in functional energy materials require in situ/operando techniques which limit the use of structural and functional characterization techniques that provide local information. Here, force-based atomic force microscopies (AFMs) have provided novel insights into locally probing electrochemical mechanisms on tens of nanometer and even molecular length scales and provide a viable pathway to probe electrochemical processes in situ/operando. In this review, we highlight the contributions in the development and application of force-based AFM methods to elucidate the local charge storage mechanism in a variety of energy-related materials. We will focus in particular on methods or AFM modalities in a liquid electrolyte environment.

25 ENERGY STORAGE↗

Automated Experiments of Local Non–Linear Behavior in Ferroelectric Materials

An automated experiment in multimodal imaging to probe structural, chemical, and functional behaviors in complex materials and elucidate the dominant physical mechanisms that control device function is developed and implemented. Here, the emergence of non-linear electromechanical responses in piezoresponse force microscopy (PFM) is explored. Non-linear responses in PFM can originate from multiple mechanisms, including intrinsic material responses often controlled by domain structure, surface topography that affects the mechanical phenomena at the tip-surface junction, and the presence of surface contaminants. Using an automated experiment to probe the origins of non-linear behavior in ferroelectric lead titanate (PTO) and ferroelectric Al 0.93 B 0.07 N films, it is found that PTO shows asymmetric nonlinear behavior across a/c domain walls and a broadened high nonlinear response region around c/c domain walls. In contrast, for Al 0.93 B 0.07 N, well-poled regions show high linear piezoelectric responses, when paired with low non-linear responses regions that are multidomain show low linear responses and high nonlinear responses. It is shown that formulating dissimilar exploration strategies in deep kernel learning as alternative hypotheses allows for establishing the preponderant physical mechanisms behind the non-linear behaviors, suggesting that automated experiments can potentially discern between competing physical mechanisms. Furthermore, this technique can also be extended to electron, probe, and chemical imaging.

36 MATERIALS SCIENCE↗

Plasma-Assisted Epitaxy of Piezoelectric Sc x Al 1-x N Films on Sapphire for Use in Harsh-Environment Microwave Acoustic Sensors

The Sc x Al 1-x N wurtzite structure has been shown theoretically and experimentally to exhibit significantly higher piezoelectric coupling compared to pure AlN. In this work, a plasma-assisted epitaxial growth method has been used to synthesize epitaxial (0002) Sc x Al 1-x N films on c-sapphire substrates from x = 0.07 to 0.30 by co-evaporating high-purity Sc and Al sources in the presence of a nitrogen plasma generated by an RF plasma source. Epitaxial Sc x Al 1-x N films with highly oriented (0002) grains and in-plane registry were produced on c-sapphire substrates that were pre-exposed to the nitrogen plasma to form an oxynitride seed layer. Growth of Sc x Al 1-x N films was carried out at 930°C under both metal-rich and N-rich conditions using precisely controlled Sc, Al, and N-plasma fluxes. Metal-rich depositions yielded non-(0002)-oriented Sc x Al 1-x N grains and intermetallic ScAl grains. Nitrogen-rich growth with a Sc/Al flux ratio of 1/3 produced the best (0002) epitaxy as determined by x-ray diffraction analysis. Surface acoustic wave resonator (SAWR) devices were fabricated from 500-nm-thick Sc x Al 1-x N and AlN films to extract their electromechanical coupling coefficients, k 2 . As the Sc concentration in the films increases, the degree of (0002) epitaxy is reduced, yet the value of k 2 increases becasue there is more Sc in the wurzite lattice despite the decreased level of (0002) grain alignment. As a result, the use of a 10-nm-thick Si x N y capping layer on top of the Sc x Al 1-x N films aids in preventing etching during SAWR device photolithography and also helps hinder film oxidation up to 800°C.

36 MATERIALS SCIENCE↗

A Simplified Method for Predicting Shaker Voltage in IMMATs

Impedance Matched Multi-Axis Tests (IMMATs) can replicate in-service vibration induced stress more accurately than single axis shaker table tests as they can better match a part’s operational boundary conditions and excite it in multiple degrees of freedom simultaneously. Here, the shakers used in IMMATs are less powerful than shaker tables, so shaker force limits can be exceeded during tests if they are not placed adequately for the desired environment. The ability to predict shaker voltage and force before performing a test is, therefore, helpful in selecting shaker locations so that their limits are not exceeded. In this study, electrodynamic shakers were modeled as discrete electromechanical systems, and the shaker parameters were chosen to match experimentally obtained acceleration/voltage frequency response functions (FRFs). These models were coupled to a finite element model of the device under test (DUT) via dynamic substructuring, and the substructured model was demonstrated to accurately predict shaker voltage as well as the error in reproducing the environment at multiple accelerometer locations. A simple method called the FRF Multiplication method, in which the FRF of the substructured system is approximated as the product of two separate FRFs of the shaker and DUT respectively, was proposed and applied to the same system, yielding similar voltage and error predictions to those obtained using substructuring. Simple case studies were presented to explore the applicability of the proposed method, and it was demonstrated to have similar accuracy to the substructuring method in a range of cases. Additionally, we showed that while it was not possible to derive a unique model of the shakers from acceleration/voltage FRFs alone, the models that could be obtained were sufficient to predict test error almost perfectly and shaker voltage with less than 40 percent error.

42 ENGINEERING↗

Development of a new control rod drive mechanism design for the ISU AGN-201M reactor

The Aerojet General Nucleonics (AGN) model 201-Modified, known as the AGN-201M reactor, plays an essential role in the educational and research activities at Idaho State University (ISU). The ISU AGN-201M's original Control Rod Drive Mechanism (CRDM) has been in operation for more than fifty years with no large-scale redesigns. The CRDM is required to eject the fuel rods within one second during a SCRAM event (also known as a 'reactor trip') and adjust the control rods' insertion speed, and keeps the rod insertion sequence correct. The existing control rod drive mechanisms meet these criteria but experience a few concerns due to aging. Concerns include complex maintenance and costly repairs for old electromechanical components, rod position feedback errors, and the impediment of the plate during a SCRAM due to binding of the lead screws of the existing mechanism. During a binding event, the drive mechanism becomes locked, preventing the control rod's magnetic plate from moving in or out under the reactor's normal and emergency operating conditions. Although, the binding has no effect on the ability of the rod to exit the core during the SCRAM. To counteract the concerns and issues with the current CRDM, a new design has been proposed using newer components and a simplified design. The new design utilizes more advanced electric and mechanical components that are commercially available. The new CRDM system is divided into four main aspects: (1) control rod movement design (motor, lead screw, guide rods), (2) control rod ejection (springs, electromagnet), (3) control rod position and feedback (position transducer, microswitches), and (4) material selection and structural analysis. The new design aims to reduce the overall complexity and probability of failure to improve the reactor's overall reliability. With proper material selection and improved structural design, the new drives are lighter with little to no change in structural integrity. The new control rod drive mechanism eliminates binding scenarios by using a single lead screw and implementing additional guide rods. An advanced linear position sensor and microswitches replace the existing and aging synchro system for accurate rod position feedback resulting in better reactivity control. The new design meets the reactor's operational limits by having an average reactivity insertion of 0.065% Δk/k per second, which corresponds to a total control rod insertion time of 19.23 s, while the control rod's ejection time remains less than one second during a SCRAM event. The new design ensures the reactor's long-term viability for educational and research activities by increasing the reliability and safety of operation for years to come.

21 SPECIFIC NUCLEAR REACTORS AND ASSOCIATED PLANTS↗

Using non-invasive MEMS pressure sensors for measuring building envelope air leakage

Micro-electromechanical systems (MEMS)-based sensors have seen significant improvements in accuracy and cost over the past several years, and due to the need for altitude sensing in unmanned aerial vehicles and wearable technologies, absolute pressure sensors have shown the most dramatic improvements. This paper investigates applications of MEMS sensors in commercial buildings, including pairing two absolute pressure sensors to determine differential pressures between different locations in and around buildings. Differential pressure measurements are commonly made in commercial buildings for a number of applications, including static pressure measurements for variable-speed supply fan control, air balancing in hospitals, and for envelope and duct air leakage testing. This paper focuses specifically on envelope air-leakage testing applications of these sensors. The use of continuous pressure measurements in addition to one-time non-intrusive outdoor airflow measurements of rooftop packaged units is investigated. A comparison with standardized leakage testing indicated that continuous measurements with MEMS pressure-sensors were able to estimate envelope leakage to within 3–16% of the standardized test result. In addition, the magnitude and stability of differential pressure differences that can be resolved with absolute pressure sensors are also investigated in the laboratory and the field. Results show that the sensors can be effectively used for pressures seen in low rise buildings with rooftop units.

32 ENERGY CONSERVATION, CONSUMPTION, AND UTILIZATI↗

Thermal and electric multidomain dynamic model for integration of power grid distribution with behind-the-meter devices

As renewable energy sources like solar and wind power become more integrated into the grid, coordinated control of behind-the-meter devices is crucial for enhancing grid flexibility and reliability and for meeting cost targets, with standardized models being developed to support this transition. The increasing flexibility and uncertainty of integrated renewable energy grids, along with interactions between various subsystems, make traditional steady-state modeling insufficient to capture transient and dynamic behaviors. Current models (e.g., composite load and battery equivalent models) focus on thermodynamic or electrical characteristics but overlook critical electromechanical interactions. This limits the ability to share performance information for grid services and hampers fast dynamic simulations. In addition, motor stalling is usually triggered by a fault event and attributed to the characteristics of the mechanical torque of the motor, resulting in absorption of a large amount of reactive power during the stalling period. Further, this significant withdrawal of reactive power will deteriorate the dynamic voltage stability of power grids and cause delayed voltage recovery. Therefore, an in-depth modeling of the thermodynamics or mechanical torque is essential to study the impacts of the realistic torque characteristics of those behind-the-meter devices on power system voltage stability. This study developed a dynamic multidomain model for building HVAC systems, such as air-source heat pumps, to simulate their thermal and electrical responses to grid transients. The model can accurately predict power metrics with a mean absolute percentage error of 10%, by validating against with power system computer-aided design performance data. Case studies demonstrate the model capability of capturing the transient response to sudden voltage changes, rapid load fluctuations, and system shutdowns respectively. During a sudden voltage drop (30% for 0.1s), a fully loaded heat pump’s motor speed dropped, continued declining, and shut down after 3.6s, with severe power oscillations and a torque spike. A partially loaded unit experienced temporary oscillations but stabilized. Under higher building loads, compressor speed increased from 64% to 100%, with power and torque rising before stabilizing. In safety-triggered shutdowns, power decreased after minor fluctuations, and torque briefly spiked before dropping to zero.

24 POWER TRANSMISSION AND DISTRIBUTION↗