In the past few years,the theory of thermal transport in amorphous solids has been substantially extended beyond the Allen-Feldman model.The resulting formulation,based on the Green-Kubo linear response or the Wigner-...In the past few years,the theory of thermal transport in amorphous solids has been substantially extended beyond the Allen-Feldman model.The resulting formulation,based on the Green-Kubo linear response or the Wigner-transport equation,bridges this model for glasses with the traditional Boltzmann kinetic approach for crystals.The computational effort required by these methods usually scales as the cube of the number of atoms,thus severely limiting the size range of computationally affordable glass models.Leveraging hydrodynamic arguments,we show how this issue can be overcome through a simple formula to extrapolate a reliable estimate of the bulk thermal conductivity of glasses from finite models of moderate size.We showcase our findings for realistic models of paradigmatic glassy materials.展开更多
Despite governing heat management in any realistic device,the microscopic mechanisms of heat transport in all-solid-state electrolytes are poorly known:existing calculations,all based on simplistic semi-empirical mode...Despite governing heat management in any realistic device,the microscopic mechanisms of heat transport in all-solid-state electrolytes are poorly known:existing calculations,all based on simplistic semi-empirical models,are unreliable for superionic conductors and largely overestimate their thermal conductivity.In this work,we deploy a combination of state-of-the-art methods to calculate the thermal conductivity of a prototypical Li-ion conductor,the Li_(3)ClO antiperovskite.By leveraging ab initio,machine learning,and force-field descriptions of interatomic forces,we are able to reveal the massive role of anharmonic interactions and diffusive defects on the thermal conductivity and its temperature dependence,and to eventually embed their effects into a simple rationale which is likely applicable to a wide class of ionic conductors.展开更多
基金This work was partially funded by the EU through the MAX Centre of Excellence for supercomputing applications(Project No.10109337)the Italian Ministry of Research and Education through by the Italian MUR through the PRIN 2017 FERMAT(grant No.2017KFY7XF)by the National Centre from HPC,Big Data,and Quantum Computing(grant No.CN00000013).
文摘In the past few years,the theory of thermal transport in amorphous solids has been substantially extended beyond the Allen-Feldman model.The resulting formulation,based on the Green-Kubo linear response or the Wigner-transport equation,bridges this model for glasses with the traditional Boltzmann kinetic approach for crystals.The computational effort required by these methods usually scales as the cube of the number of atoms,thus severely limiting the size range of computationally affordable glass models.Leveraging hydrodynamic arguments,we show how this issue can be overcome through a simple formula to extrapolate a reliable estimate of the bulk thermal conductivity of glasses from finite models of moderate size.We showcase our findings for realistic models of paradigmatic glassy materials.
基金This work was partially funded by the EU through the MAX Centre of Excellence for supercomputing applications(Project No.824143)the Italian Ministry of Research and education through the PRIN 2017 FERMAT grant.F.G.acknowledges funding from the Swiss National Science Foundation(SNSF),through Project No.200021-182057from the European Union’s Horizon 2020 research and innovation programme under the Marie Skłodowska-Curie Action IF-EF-ST,grant agreement No.101018557(TRANQUIL)。
文摘Despite governing heat management in any realistic device,the microscopic mechanisms of heat transport in all-solid-state electrolytes are poorly known:existing calculations,all based on simplistic semi-empirical models,are unreliable for superionic conductors and largely overestimate their thermal conductivity.In this work,we deploy a combination of state-of-the-art methods to calculate the thermal conductivity of a prototypical Li-ion conductor,the Li_(3)ClO antiperovskite.By leveraging ab initio,machine learning,and force-field descriptions of interatomic forces,we are able to reveal the massive role of anharmonic interactions and diffusive defects on the thermal conductivity and its temperature dependence,and to eventually embed their effects into a simple rationale which is likely applicable to a wide class of ionic conductors.
