Two-Dimensional 109Ag NMR and Random-Walk Simulation Studies of Silver Dynamics in Glassy Silver Ion Conductors

Vogel, Michael; Brinkmann, Christian; Eckert, Hellmut; Heuer, Andreas

doi:10.1006/snmr.2002.0089

Cited by 23 publications

(43 citation statements)

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“…Figure 1 shows temperature-dependent 109 Ag NMR spectra of AgI 0.3 -(AgPO 3 ) 0.7 glass, which are typical of results for silver iodide doped silver phosphate glasses [20,22]. We see that the spectra at sufficiently low and high temperatures are well described by a broad Gaussian and a narrow Lorentzian, respectively.…”

Section: Line-shape Analysismentioning

confidence: 60%

“…reflecting the slow ions [22]. Furthermore, 6 Li and 7 Li NMR spectra comprising broad Gaussian and narrow Lorentzian components were reported for glassy lithium ion conductors [1,18].…”

Section: Line-shape Analysismentioning

confidence: 96%

“…At intermediate temperatures, the 109 Ag NMR line shapes of glassy silver ion conductors were well described by a weighted superposition of a broad Gaussian and a narrow Lorentzian, indicating that slow (τ 10 μs) and fast (τ 10 μs) silver ions coexist [20,22,27]. In this range, cooling resulted in a continuous decrease of the relative intensity of the Lorentzian, as can be seen for the example of AgI 0.3 -(AgPO 3 ) 0.7 glass in Fig.…”

Section: Line-shape Analysismentioning

confidence: 99%

“…In detail, (i) ions that occupy the same or periodic sites at the beginning and at the end of the mixing time do contribute since, within experimental resolution, the frequencies are identical at equivalent sites, (ii) ions that reside at different sites, on average, do not contribute, and (iii) rearrangements of neighboring ions have no effect, i.e., single-particle correlations functions are measured. In 109 Ag NMR work on glassy and crystalline silver ion conductors, Δω i typically exceeds Δω d by about 3 orders of magnitude so that the above condition can be met [20][21][22][23][24][25][26][27]. Specifically, all 109 Ag NMR MT-CF of the present contribution were measured using an evolution time t p = 100μs.…”

Section: Analysis and Interpretationmentioning

confidence: 99%

“…2.2.1. We exploited the potential of 109 Ag NMR 2T-CF to characterize silver ion dynamics in various materials [20][21][22][23]25]. It was found that the temperature dependence of 109 Ag NMR Fig.…”

Section: Nmr Two-time Correlation Functionsmentioning

confidence: 99%

See 4 more Smart Citations

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: Line-shape Analysismentioning

confidence: 60%

“…reflecting the slow ions [22]. Furthermore, 6 Li and 7 Li NMR spectra comprising broad Gaussian and narrow Lorentzian components were reported for glassy lithium ion conductors [1,18].…”

Section: Line-shape Analysismentioning

confidence: 96%

Section: Line-shape Analysismentioning

confidence: 99%

Section: Analysis and Interpretationmentioning

confidence: 99%

Section: Nmr Two-time Correlation Functionsmentioning

confidence: 99%

See 3 more Smart Citations

NMR Multi-Time Correlation Functions of Ion Dynamics in Solids

Brinkmann

Faske

Koch

et al. 2010

Zeitschrift Für Physikalische Chemie

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From Micro to Macro: Access to Long‐Range Li⁺ Diffusion Parameters in Solids via Microscopic ^6, 7Li Spin‐Alignment Echo NMR Spectroscopy

2011

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The development of highly conductive solids is a rapidly growing research area in materials science. In particular, the study of Li-ion conductors is driven by the ambitious effort to design powerful lithium-ion batteries. A deeper understanding of Li dynamics in solids requires the availability of a large set of complementary techniques to probe Li self-diffusion on different length and time-scales. We report on (7)Li as well as (6)Li spin-alignment echo (SAE) nuclear magnetic resonance (NMR) spectroscopy, which is capable of probing long-range diffusion parameters from a microscopic, that is, atomic-scale, point of view. So far, variable-temperature SAE NMR spectroscopy has been applied to a number of polycrystalline and glassy Li-ion conductors. The materials investigated serve as model systems to unravel the interesting features of the technique in determining reliable Li jump rates and hopping activation energies. In particular, the latter are compared with those probed by macroscopic techniques such as dc-conductivity measurements that are sensitive to long-range translational motions.

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On the lifetime of dynamical heterogeneities associated with the ionic jump motion in glasses: Results from molecular dynamics simulations and NMR experiments

Vogel

Brinkmann

Eckert

et al. 2006

Journal of Non-Crystalline Solids

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Two-Dimensional 109Ag NMR and Random-Walk Simulation Studies of Silver Dynamics in Glassy Silver Ion Conductors

Cited by 23 publications

References 50 publications

NMR Multi-Time Correlation Functions of Ion Dynamics in Solids

NMR Multi-Time Correlation Functions of Ion Dynamics in Solids

From Micro to Macro: Access to Long‐Range Li⁺ Diffusion Parameters in Solids via Microscopic ^6, 7Li Spin‐Alignment Echo NMR Spectroscopy

On the lifetime of dynamical heterogeneities associated with the ionic jump motion in glasses: Results from molecular dynamics simulations and NMR experiments

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Two-Dimensional 109Ag NMR and Random-Walk Simulation Studies of Silver Dynamics in Glassy Silver Ion Conductors

Cited by 23 publications

References 50 publications

NMR Multi-Time Correlation Functions of Ion Dynamics in Solids

NMR Multi-Time Correlation Functions of Ion Dynamics in Solids

From Micro to Macro: Access to Long‐Range Li+ Diffusion Parameters in Solids via Microscopic 6, 7Li Spin‐Alignment Echo NMR Spectroscopy

On the lifetime of dynamical heterogeneities associated with the ionic jump motion in glasses: Results from molecular dynamics simulations and NMR experiments

Contact Info

Product

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From Micro to Macro: Access to Long‐Range Li⁺ Diffusion Parameters in Solids via Microscopic ^6, 7Li Spin‐Alignment Echo NMR Spectroscopy