Replication Data for: Tailoring Li-Al-O Interphases in Garnet-Type Solid-State Electrolytes via Powder Atomic Layer Depositiondoi:10.26165/JUELICH-DATA/1XFQBWJülich DATA2026-03-091Steinhoff, Michael; Domgans, Anna; Ahmed, Jehad; Schierholz, Roland; Daniel, Davis Thomas; Aghdassi, Nabi; Yu, Shicheng; Tempel, Hermann; Eichel, Rüdiger-A., 2026, "Replication Data for: Tailoring Li-Al-O Interphases in Garnet-Type Solid-State Electrolytes via Powder Atomic Layer Deposition", https://doi.org/10.26165/JUELICH-DATA/1XFQBW, Jülich DATA, V1Replication Data for: Tailoring Li-Al-O Interphases in Garnet-Type Solid-State Electrolytes via Powder Atomic Layer Depositiondoi:10.26165/JUELICH-DATA/1XFQBWSteinhoff, MichaelDomgans, AnnaAhmed, JehadSchierholz, RolandDaniel, Davis ThomasAghdassi, NabiYu, ShichengTempel, HermannEichel, Rüdiger-A.Steinhoff, MichaelDomgans, AnnaAhmed, JehadSchierholz, RolandDaniel, Davis ThomasAgdhassi, NabiYu, ShichengTempel, HermannEichel, Rüdiger-A.VeloxTopSpinCasaXPSDiffrac.TopasAztecEC-LabZview1703FI1213XPO510AJülich DATASteinhoff, MichaelTempel, HermannSteinhoff, Michael2025-09-18Chemistry<h2>Study Overview</h2> <p> In this study, the influence of atomic layer deposition (ALD) derived Li-Al-O interphases in garnet-type Li_6.4La₃Zr_1.4Ta_0.6O₁₂ (LLZTO) solid-state electrolyte (SSE) was investigated. Garnet-type SSE are prone to lithium dendrite growth along interfaces, which causes short-circuits, significantly reducing cell performance. ALD offers high control over coating chemistry and morphology to precisly modify these interfaces in SSEs. Here, Al₂O₃ ALD coatings were applied on LLZTO powder. MAS NMR, XPS and STEM analysis reveal the formation of a compositionally graded Li-Al-O interphase upon deposition due to proton-exchange-induced lithium diffusion. During high-temperature sintering, the ALD coating induces densification and considerable interdiffusion with LLZTO, resulting in a multi-phase microstructure which can be directly controlled via the ALD process, as confirmed by XRD, SEM and EDS measurments. Electrochemical testing reveals that medium-thickness coatings (~ 6.8 nm, 25 ALD cycles) yield optimal performance, exhibiting ionic conductivity at room temperature of 0.39 mS/cm with good Li-dendrite resitance and long-term cycling stability. </p> <hr> <h2>Dataset Description</h2> <p> This dataset contains NMR, XPS, XRD, Ellipsometry, EDS line scans, and electrochemical measurements to investigate Li-Al-O interphases in LLZTO. </p> <p> The dataset is organized into the following folders: </p> <dl> <dt><strong>NMR</strong></dt> <dd> ²⁷Al Solid-state magic angle spinning nuclear magnetic resonance (MAS NMR) spectroscopy experiments were performed using an AvanceNEO spectrometer (Bruker). Data are stored in the folder <code>NMR</code>. </dd> <dt><strong>XPS</strong></dt> <dd> X-ray photoelectron spectroscopy (XPS) measurements of the Al 2p and C 1s region were conducted using a NEXSA G2 spectrometer (Thermo Fisher Scientific). Data are stored in the folder <code>XPS</code>. </dd> <dt><strong>XRD</strong></dt> <dd> X-ray diffraction (XRD) experiments were recorded using an Empyrean diffractometer (Pananalytical). Quantitative phase analysis (QPA) on the XRD diffractograms were conducted using the software package Diffrac.Topas version 7 (Bruker). The corresponding diffractograms and fitting data are stored in the folder <code>XRD</code>. </dd> <dt><strong>Ellipsometry</strong></dt> <dd> Ellipsometry data were recorded using a FS-8 spectroscopic ellipsometer (Film Sense LLC). Data are stored in the folder <code>Ellipsometry</code>. </dd> <dt><strong>Electrochemistry</strong></dt> <dd> Electrochemical impedance spectroscopy (EIS), critical current density (CCD) measurements, long-term plating/stripping experiments and chronoamperometry (CA) measurements were performed. Data are stored in the folder <code>Electrochemistry</code>. </dd> <dt><strong>EDS line profile</strong></dt> <dd> EDS line profiles were recorded using a FEI Titan G2 80-200 CREWLEY system. Data are stored in the folder <code>EDS_line_profile</code>. </dd> </dl>Al2O3_reference_NMR.txttext/plainAl2O3_reference_XPS_Al2p.txttext/plainEC_README.txttext/plainEDS_README.txttext/plainEllipsometry_README.txttext/plainLiAlO2_reference_NMR.txttext/plainLiAlO2_reference_XPS_Al2p.txttext/plainLLZTO_100cycles_CA_1.txttext/plainLLZTO_100cycles_CA_2.txttext/plainLLZTO_100cycles_CCD.txttext/plainLLZTO_100cycles_EIS.txttext/plainLLZTO_100cycles_Longterm.txttext/plainLLZTO_100cycles_NMR.txttext/plainLLZTO_100cycles_QPA_fit.txttext/plainLLZTO_100cycles_QPA_plot.txttext/plainLLZTO_100cycles_XPS_Al2p.txttext/plainLLZTO_100cycles_XRD.txttext/plainLLZTO_10cycles_CA_1.txttext/plainLLZTO_10cycles_CA_2.txttext/plainLLZTO_10cycles_CCD.txttext/plainLLZTO_10cycles_EIS.txttext/plainLLZTO_10cycles_Longterm.txttext/plainLLZTO_10cycles_QPA_fit.txttext/plainLLZTO_10cycles_QPA_plot.txttext/plainLLZTO_10cycles_XRD.txttext/plainLLZTO_25cycles_CA_1.txttext/plainLLZTO_25cycles_CA_2.txttext/plainLLZTO_25cycles_CCD.txttext/plainLLZTO_25cycles_EIS.txttext/plainLLZTO_25cycles_Longterm.txttext/plainLLZTO_25cycles_QPA_fit.txttext/plainLLZTO_25cycles_QPA_plot.txttext/plainLLZTO_25cycles_XRD.txttext/plainLLZTO_50cycles_CA_1.txttext/plainLLZTO_50cycles_CA_2.txttext/plainLLZTO_50cycles_CCD.txttext/plainLLZTO_50cycles_EIS.txttext/plainLLZTO_50cycles_Longterm.txttext/plainLLZTO_50cycles_QPA_fit.txttext/plainLLZTO_50cycles_QPA_plot.txttext/plainLLZTO_50cycles_XRD.txttext/plainLLZTO_Pristine_QPA_fit.txttext/plainLLZTO_Pristine_QPA_plot.txttext/plainLLZTO_pristine_XPS_C1s.txttext/plainLLZTO_Pristine_XRD.txttext/plainLong_range_Al.txttext/plainLong_range_La.txttext/plainLong_range_O.txttext/plainLong_range_Ta.txttext/plainLong_range_Zr.txttext/plainNMR_README.txttext/plainREADME.txttext/plainShort_range_Al.txttext/plainShort_range_BF.txttext/plainShort_range_La.txttext/plainShort_range_O.txttext/plainShort_range_Ta.txttext/plainShort_range_Zr.txttext/plainSi_reference_100cycles_Ellipsometry_1.txttext/plainSi_reference_100cycles_Ellipsometry_2.txttext/plainSi_reference_100cycles_Ellipsometry_3.txttext/plainXPS_README.txttext/plainXRD_README.txttext/plain