P1-3168Microscopic Insights into the Interfacial Kinetics of Li1+xAlxTi2−x(PO4)3 (LATP) During Solid-State Reaction via ReaxFF-MD Simulation：：AllsolidReaxFFOurresearchaddressestheurgentneedforsafer,high-performanceenergystoragebyimprovingsolidelectrolytesinnext-generationall-solid-stateLi-ionbatteries.ByreducingphasevariabilityinLi₁₊ₓAlₓTi₂₋ₓ(PO₄)₃,weaimtoenhanceionicconductivityandstability,directlysupportingcleanerenergysystemsandsustainableelectrificationdemands.oOxygen-terminatedLATP|LTPandLTP|AlPO₄high-indexinterfacesexhibitthehighestiondiffusivity.oElevatedtemperaturesdriveAlmigrationandpolyhedraltransformations-criticalforLATPphaseformationinASSBs.Ion Transport Properties, Effect of Al on Ion Dynamics at Interface•ExtendMDsimulationstolongertimescalesandlargersystemsforbettercapturingsynthesisdynamics.•CorrelatesimulationinsightswithexperimentalsynthesistoguidescalableASSBelectrolytedesign.IntroductionHigh-temperature synthesis of LATP often leads to unwanted secondary phases and non-optimal AI distribution, lowering ionic conductivity.ReaxFF-based MD simulations probe interfacial ion transport and structural transformations at LATP|LTP and LTP|AlPO₄ contacts.Enables control of interface kinetics for tailored microstructures in ASSBs, though simulations are limited by time/length scales.Theme underDiscussionAtomic structures of LTP|LATP and LTP|AlPO₄ with high-and low-index interfaces framework (1.2 Å separation). Li (blue), P (cyan), Ti (green), Al (orange), O (red).2ReaxFF-MDiontrajectories(1600K,500ps)atLTP|LATPandLTP|AlPO₄high-indexinterfaces.Resultsshownfororiginaland10%expandedcells:(left)O₂(LTP)|O₂(LATP),(right)Al₂P₂O₃(AlPO₄)|O₂(LTP).ColorgradientshighlightmigrationofLi,Ti,Al,P,andO,withinterfacialzonesoutlinedbydashedboxes.3Species-resolvedtotalMSDs(Li,Ti,P,O,Al)atInterface1ofLTP|LATP(left)andLTP|AlPO₄(right)fromReaxFF-MDat1600K(500ps),comparinghigh-andlow-indexion-terminatedinterfaces.4ApparenttotalMSDofionsatInterface1for(a)LTP|LATPand(b)LTP|AlPO₄fromReaxFF-MDat1600K(500ps),comparingnoexpansion(black),5%(red),and10%(green).Left: RDF (g(r)) and RCN (C(r)) for P–O pairs (top) and time evolution of PO₃, PO₄, PO₅ units (bottom) in LTP|LATP and LTP|AlPO₄ at 1600 K (500 ps). Right: RDF/RCN for Ti–O pairs (top) and evolution of TiO₃, TiO₄, TiO₅, TiO₆ units (bottom) under the same conditions.SLeft:TemporalevolutionofP–O–P,Ti–O–Ti,P–O–Ti(corner),andP–O–Ti(edge)linkagesatLTP|LATP(a)andLTP|AlPO₄(c)interfaces,obtainedfroma100psheatingphase(300–1600K)followedby500psReaxFF-MDat1600K(unexpanded).Dataaveragedevery5pswitherrorsinred.Right:MDsnapshotsofM1–O–M2(M=P,Ti)linkagesatLTP|LATP(b)andLTP|AlPO₄(d)interfacesatselectedtimes.7Left:AliontrajectoriesattheLTP|AlPO₄interfacewith10%expansionfromReaxFF-MDat1600K(top)and2400K(bottom).Right:EvolutionofAl–OpolyhedrainbulkLTPat2400K,withinsetshowingAlO₃(red),AlO₄(green),andAlO₅(blue);dataaveragedevery5ps,errorsincyan.8Left:AtomisticmodelofLTP|LATPcontact(x=0.3AlinLATP)andAl-iontrajectoriesat2400K.Right:TimeevolutionofAl-ioncountsinLATPandLTPduringheating(300–2400K,0.5ns)andproduction(2nsat2400K);dottedblueboxmarksequalization(2Alineachregion).
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