Atomic-scale measurement of ultraslow Li motions in glassy<mml:math xmlns:mml="http://www.w3.org/1998/Math/MathML" display="inline"><mml:mrow><mml:msub><mml:mrow><mml:mtext>LiAlSi</mml:mtext></mml:mrow><mml:mn>2</mml:mn></mml:msub><mml:msub><mml:mtext>O</mml:mtext><mml:mn>6</mml:mn></mml:msub></mml:mrow></mml:math>by two-time<mml:math xmlns:mml="http://www.w3.org/1998/Math/MathML" display="inline"><mml:mrow><mml:mmultiscripts><mml:mtext>L</mml:mtext><mml:mprescripts /><mml:none /><mml:mn>6</mml:mn></mml:mm

Wilkening, Martin; Kuhn, Alexander; Heitjans, Paul

doi:10.1103/physrevb.78.054303

Cited by 59 publications

(56 citation statements)

References 69 publications

(129 reference statements)

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“…6 Li and 7 Li NMR stimulated-echo experiments proved a versatile tool to study lithium ionic motion in solids [1,15,17,18,[34][35][36][37][38]. For these nuclei, Li−Li DD interactions can facilitate spin diffusion.…”

Section: Nmr Two-time Correlation Functionsmentioning

confidence: 99%

NMR Multi-Time Correlation Functions of Ion Dynamics in Solids

Brinkmann

Faske

Koch

et al. 2010

Zeitschrift Für Physikalische Chemie

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We show that NMR multi-time correlation functions provide interesting new insights into the nature of lithium and silver ion dynamics in solids. For solid ion conductors, they usually probe the elementary jumps of the long-range charge transport. NMR two-time correlation functions yield rates and activation energies of the ionic hopping motion. Moreover, they reveal that the ionic relaxation exhibits a strong nonexponentiality in the studied crystals and glasses. NMR three-time correlation functions enable quantitative determination of the origin of the nonexponentiality. For various solid-state electrolytes, the analysis shows that pronounced dynamical heterogeneities govern the ionic hopping motion. If dynamical heterogeneities exist, NMR four-time correlation functions allow one to measure the time scale of exchange processes within the rate distributions. For silver ion dynamics in a crystalline and a glassy material, the results indicate that initially slow ions exhibit random new rates from broad rate distributions after very few jump events.

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Section: Nmr Two-time Correlation Functionsmentioning

confidence: 99%

NMR Multi-Time Correlation Functions of Ion Dynamics in Solids

Brinkmann

Faske

Koch

et al. 2010

Zeitschrift Für Physikalische Chemie

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“…By investigating the Li dynamics in the crystal and in the corresponding glass, being chemically identical but structurally different, it is possible to deduce some structural features which promote ionic motion. Comparisons between diffusivities in crystalline spodumene as well as other Li aluminosilicates and their respective glassy counterparts have been reported in [13,14,[17][18][19][20][21][22][23][24][25]. When nanostructured samples are considered, in addition to the two structural varieties glass and crystal many other samples of the same chemical composition but with a different structure can be prepared allowing new insights into the structure-dynamics relation in those systems.…”

Section: Introductionmentioning

confidence: 99%

Li Ion Diffusion in Nanocrystalline and Nanoglassy LiAlSi₂O₆ and LiBO₂ - Structure-Dynamics Relations in Two Glass Forming Compounds

Kuhn¹,

Tobschall²,

Heitjans³

2009

Zeitschrift Für Physikalische Chemie

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In the present study the Li diffusivity in nanostructured samples of two glass forming model systems, spodumene (LiAlSi 2 O 6 ) and lithium metaborate (LiBO 2 ), was examined using 7 Li nuclear magnetic resonance (NMR) spin-lattice relaxometry and dc conductivity measurements. The nanostructured samples were prepared by high-energy ball milling of the respective crystalline starting material on the one hand and the corresponding glass on the other hand. The diffusivity of the glass exceeds that of the crystalline sample for both systems. However, when the crystalline samples are mechanically treated by ball milling the diffusivity is enhanced. Nevertheless, the diffusivity of these nanocrystalline samples remains lower than that of the corresponding glass. Surprisingly, when the glassy samples are treated in the same way the diffusivity decreases. After sufficiently long milling times the diffusivity of these nanoglassy samples approaches that of the nanocrystalline samples. This convergence effect seems to be due to structural relaxation processes as is suggested by supplementary infrared spectroscopy and 27 Al, 12B magic angle spinning NMR measurements.

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“…By sensing the dipolar-magnetic or quadrupolar-electric fluctuations as a function of temperature, through NMR relaxation techniques bulk ion dynamics are probed that shed light on the elementary steps governing ion hopping. Moreover, in ideal cases NMR also allows to draw conclusions about the underlying motional correlation functions [68][69][70][71][72]. In contrast to impedance or conductivity measurements no post-preparation of the synthesized powder, i.e., pressing of dense pellets, applying of electrodes, is necessary.…”

Section: Introductionmentioning

confidence: 99%

Ion dynamics in solid electrolytes for lithium batteries

et al. 2017

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All-solid-state batteries with ceramic electrolytes and lithium metal anodes represent an attractive alternative to conventional ion battery systems. Conventional batteries still rely on flammable liquids as electronic insulators. Despite the great efforts reported over the last years, the optimum solid electrolyte has, however, not been found yet. One of the most important properties which decides whether a ceramic is useful to work as electrolyte is ionic transport. The various time-domain nuclear magnetic resonance (NMR) techniques might help characterize and select the most suitable candidates. Together with conductivity measurements it is possible to analyze ion dynamics on different length-scales, i.e., to differentiate between local, within-site hopping processes from long-range ion transport. The latter needs to be sufficiently fast in the ceramic, in the best case competing with that of liquid electrolytes. In addition to conductivity spectroscopy, NMR can help understand the relationship between local structure and dynamic parameters. Besides information on activation energies and jump rates the data also contain suggestions about the relevant elementary steps of ion hopping and, thus, Support by the Deutsche Forschungsgemeinschaft (DFG) is highly appreciated (FOR 1277 diffusion pathways through the crystal lattice. Recent progress in characterizing ion dynamics in ceramic electrolytes by NMR relaxometry will be briefly reviewed. Focus is put on presently discussed solid electrolytes such as garnets, phosphates and sulfides, which have so far been studied in our lab.

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Atomic-scale measurement of ultraslow Li motions in glassyLiAlSi2O6by two-timeL6

Cited by 59 publications

References 69 publications

NMR Multi-Time Correlation Functions of Ion Dynamics in Solids

NMR Multi-Time Correlation Functions of Ion Dynamics in Solids

Li Ion Diffusion in Nanocrystalline and Nanoglassy LiAlSi₂O₆ and LiBO₂ - Structure-Dynamics Relations in Two Glass Forming Compounds

Ion dynamics in solid electrolytes for lithium batteries

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Atomic-scale measurement of ultraslow Li motions in glassyLiAlSi2O6by two-timeL6

Cited by 59 publications

References 69 publications

NMR Multi-Time Correlation Functions of Ion Dynamics in Solids

NMR Multi-Time Correlation Functions of Ion Dynamics in Solids

Li Ion Diffusion in Nanocrystalline and Nanoglassy LiAlSi2O6 and LiBO2 - Structure-Dynamics Relations in Two Glass Forming Compounds

Ion dynamics in solid electrolytes for lithium batteries

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Li Ion Diffusion in Nanocrystalline and Nanoglassy LiAlSi₂O₆ and LiBO₂ - Structure-Dynamics Relations in Two Glass Forming Compounds