In the context of ionic transport in solids, the variation of a migration barrier height under electric fields is traditionally assumed to be equal to the classical electric work of a point charge that carries the transport charge. However, how reliable is this phenomenological model and how does it fare with respect to Modern Theory of Polarization? In this work, we show that such a classical picture does not hold in general as collective dipole effects may be critical. Such effects are unraveled by an appropriate polarization decomposition and by an expression that we derive, which defines the equivalent polarization-work charge. The equivalent polarization-work charge is not equal neither to the transported charge, nor to the Born effective charge of the migrating atom alone, but it is defined by the total polarization change at the transition state. Our findings are illustrated by oxygen charged defects in MgO and in SiO2.

Collective dipole effects in ionic transport under electric fields / Salles, N.; Martin-Samos, L.; de Gironcoli, S.; Giacomazzi, L.; Valant, M.; Hemeryck, A.; Blaise, P.; Sklenard, B.; Richard, N.. - In: NATURE COMMUNICATIONS. - ISSN 2041-1723. - 11:(2020), pp. 1-7. [10.1038/s41467-020-17173-w]

Collective dipole effects in ionic transport under electric fields

Salles, N.;de Gironcoli, S.;Giacomazzi, L.;
2020

Abstract

In the context of ionic transport in solids, the variation of a migration barrier height under electric fields is traditionally assumed to be equal to the classical electric work of a point charge that carries the transport charge. However, how reliable is this phenomenological model and how does it fare with respect to Modern Theory of Polarization? In this work, we show that such a classical picture does not hold in general as collective dipole effects may be critical. Such effects are unraveled by an appropriate polarization decomposition and by an expression that we derive, which defines the equivalent polarization-work charge. The equivalent polarization-work charge is not equal neither to the transported charge, nor to the Born effective charge of the migrating atom alone, but it is defined by the total polarization change at the transition state. Our findings are illustrated by oxygen charged defects in MgO and in SiO2.
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Salles, N.; Martin-Samos, L.; de Gironcoli, S.; Giacomazzi, L.; Valant, M.; Hemeryck, A.; Blaise, P.; Sklenard, B.; Richard, N.
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Utilizza questo identificativo per citare o creare un link a questo documento: https://hdl.handle.net/20.500.11767/117286
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