ترغب بنشر مسار تعليمي؟ اضغط هنا

Non-Arrhenius ionic conductivities in glasses due to a distribution of activation energies

446   0   0.0 ( 0 )
 نشر من قبل Scott Beckman
 تاريخ النشر 2012
  مجال البحث فيزياء
والبحث باللغة English




اسأل ChatGPT حول البحث

Previously observed non-Arrhenius behavior in fast ion conducting glasses [textit{Phys. Rev. Lett.} textbf{76}, 70 (1996)] occurs at temperatures near the glass transition temperature, $T_{g}$, and is attributed to changes in the ion mobility due to ion trapping mechanisms that diminish the conductivity and result in a decreasing conductivity with increasing temperature. It is intuitive that disorder in glass will also result in a distribution of the activation energies (DAE) for ion conduction, which should increase the conductivity with increasing temperature, yet this has not been identified in the literature. In this paper, a series of high precision ionic conductivity measurements are reported for $0.5{Na}_{2}{S}+0.5[x{GeS}_{2}+(1-x){PS}_{5/2}]$ glasses with compositions ranging from $0 leq x leq 1$. The impact of the cation site disorder on the activation energy is identified and explained using a DAE model. The absence of the non-Arrhenius behavior in other glasses is explained and it is predicted which glasses are expected to accentuate the DAE effect on the ionic conductivity.



قيم البحث

اقرأ أيضاً

75 - Marco Bosi , Julian Fischer , 2020
A major challenge in the modeling of ionically conducting glasses is to understand how the large variety of possible chemical compositions and specific structural properties influence ionic transport quantities. Here we revisit and extend a theoretic al approach for alkali borophosphate glasses, where changes of conductivity activation energies with the borate to phosphate mixing ratio are related to modifications of the ionic site energy landscape. The landscape modifications are caused by varying amounts of different units forming the glassy network, which lead to spatial redistributions of the counter-charges of the mobile alkali ions. Theoretical approaches are presented to calculate variations of both network former unit concentrations and activation energies with the glass composition. Applications to several alkali borophosphate glasses show good agreement with experimental data.
It is generally believed that the intrinsic properties of glasses are intimately related to potential energy landscapes (PELs). However, little is known about the PELs of glasses below the glass transition temperature (T_g). Taking advantage of lower potential energy barriers in nano systems, we have systematically investigated the dynamics behavior of two nano glasses, Al43 and Al46. Structure transformation is identified in our pure molecular-dynamics simulation far below T_g, which manifests the existence of metabasins in PELs. Surprisingly, we find that the distribution of potential energies shows a paired-Gaussian and long-tailed distribution at temperatures below and approaching T_g, correspondingly the distribution of the {alpha}-relaxation time exhibits an exponential decay. In contrast to the Gaussian distribution of energy in typical liquids and solids, the paired-Gaussian and long-tailed distribution of potential energies, as well as the exponential distribution of the {alpha}-relaxation time, may be considered as the intrinsic feature of a glass or supercooled liquid. The current results are important not only for checking the reliability of various PEL-based models, but also for exploring the microscopic nature of glasses.
123 - C. M. Jaworski , J. Yang , S. Mack 2011
Here we report on measurements of the spin-Seebeck effect of GaMnAs over an extended temperature range alongside the thermal conductivity, specific heat, magnetization, and thermoelectric power. The amplitude of the spin-Seebeck effect in GaMnAs scal es with the thermal conductivity of the GaAs substrate and the phonon-drag contribution to the thermoelectric power of the GaMnAs, demonstrating that phonons drive the spin redistribution. A phenomenological model involving phonon-magnon drag explains the spatial and temperature dependence of the measured spin distribution.
The $10$ GHz microwave conductivity, $sigma(T)$ and high field, $222$ GHz electron spin resonance (HF-ESR) of Li$_4$C$_{60}$ fulleride is measured in a wide temperature range. We suggest that the majority of ESR active sites and at least some of the charge carriers for $sigma(T)$ are electrons bound to a small concentration of surplus or vacancy ions in the polymer phase. Both $sigma(T)$ and the ESR line shape depend on ionic motion. A change of the activation energy of $sigma(T)$ at $125$ K coincides with the onset of the ionic DC conductivity. The ESR line shape is determined mainly by Li ionic motion within octahedral voids below $150$ K. At higher temperatures, fluctuations due to ionic diffusion change the environment of defects from axial to effectively isotropic on the ESR time scale. $sigma(T)$ data up to $700$ K through the depolymerization transition confirm that the monomeric phase of Li$_4$C$_{60}$ is a metal.
Thouless quantization of adiabatic particle transport permits to associate an integer topological charge with each atom of an electronically gapped material. If these charges are additive and independent of atomic positions, they provide a rigorous d efinition of atomic oxidation states and atoms can be identified as integer-charge carriers in ionic conductors. Whenever these conditions are met, charge transport is necessarily convective, i.e. it cannot occur without substantial ionic flow, a transport regime that we dub trivial. We show that the topological requirements that allow these conditions to be broken are the same that would determine a Thouless pump mechanism if the system were subject to a suitably defined time-periodic Hamiltonian. The occurrence of these requirements determines a non-trivial transport regime whereby charge can flow without any ionic convection, even in electronic insulators. These results are first demonstrated with a couple of simple molecular models that display a quantum pump mechanism upon introduction of a fictitious time dependence of the atomic positions along a closed loop in configuration space. We finally examine the impact of our findings on the transport properties of non-stoichiometric alkali-halide melts, where the same topological conditions that would induce a quantum pump mechanism along certain closed loops in configuration space also determine a non-trivial transport regime such that most of the total charge current results to be uncorrelated from the ionic ones.
التعليقات
جاري جلب التعليقات جاري جلب التعليقات
سجل دخول لتتمكن من متابعة معايير البحث التي قمت باختيارها
mircosoft-partner

هل ترغب بارسال اشعارات عن اخر التحديثات في شمرا-اكاديميا