Enhanced Adhesion Energy at Oxide/Ag Interfaces for Low-Emissivity Glasses: Theoretical Insight into Doping and Vacancy Effects
David Cornil, Nicolas Rivolta, Virginie Mercier, Hughes Wiame, David Beljonne, Jérôme Cornil
Abstract
Low-emissivity glasses rely on multistacked architectures with a thin silver layer sandwiched between oxide layers. The mechanical stability of the silver/oxide interfaces is a critical parameter that must be maximized. Here, we demonstrate by means of quantum-chemical calculations that a low work of adhesion at interfaces can be significantly increased via doping and by introducing vacancies in the oxide layer. For the sake of illustration, we focus on the ZrO2(111)/Ag(111) interface exhibiting a poor adhesion in the pristine state and quantify the impact of introducing n-type dopants or p-type dopants in ZrO2 and vacancies in oxygen atoms (nVO; with n = 1, 2, 4, 8, 10, 16), zirconium atoms (mVZr; with m = 1, 2, 4, 8), or both (nVO + mVZr; with m/n = 1:2, 1:4, 2:2, 2:4). In the case of doping, interfacial electron transfer promotes an increase in the work of adhesion, from initially 0.16 to ∼0.8 J m–2 (n-type) and ∼2.0 J m–2 (p-type) at 10% doping. A similar increase in the work of adhesion is obtained by introducing vacancies, e.g., VO [VZr] in the oxide layer yields a work of adhesion of ∼1.5–2.0 J m–2 at 10% vacancies. An increase is also observed when mixing VO and VZr vacancies in a nonstoichiometric ratio (nVO + mVZr; with 2n ≠ m), while a stoichiometric ratio of VO and VZr has no impact on the interfacial properties.