标题： 通过异价掺杂和热大气历史控制六方锰氧化物的电子性质 显示英文标题

标题： Controlling electronic properties of hexagonal manganites through aliovalent doping and thermoatmospheric history

摘要： 六边形锰氧化物家族因其多铁性、磁电耦合、非本征铁电性、功能域壁和与拓扑相关的尺度行为而受到广泛研究。已确定这些物理性质由阳离子亚晶格共同决定，而且异价掺杂可以轻易被用来修改它们。然而，掺杂也会影响阴离子缺陷化学和半导体特性，这使得该系统对合成和加工条件非常敏感。在此，我们结合密度泛函理论计算与热电和热重测量，研究了YMnO3的电子性质作为异价阳离子掺杂和热大气历史的函数。我们表明，通过异价阳离子掺杂剂和阴离子缺陷可以控制载流子浓度和输运特性，从而实现n型和p型导电性的可逆切换。这种可调性对于六边形锰氧化物在下一代电容器和域壁纳米电子学中的设想应用，或作为燃料电池或电解器中的催化剂或电极具有重要意义。此外，我们的方法可应用于其他过渡金属氧化物，为控制其半导体特性提供一般性指导。 显示英文摘要

摘要： The family of hexagonal manganites is intensively studied for its multiferroicity, magnetoelectric coupling, improper ferroelectricity, functional domain walls, and topology-related scaling behaviors. It is established that these physical properties are co-determined by the cation sublattices and that aliovalent doping can readily be leveraged to modify them. The doping, however, also impacts the anion defect chemistry and semiconducting properties, which makes the system highly sensitive to the synthesis and processing conditions. Here, we study the electronic properties of YMnO3 as function of aliovalent cation doping and thermoatmospheric history, combining density functional theory calculations with thermopower and thermogravimetric measurements. We show that the charge carrier concentration and transport properties can be controlled via both aliovalent cation dopants and anion defects, enabling reversible switching between n-type and p-type conductivity. This tunability is of importance for envisaged applications of hexagonal manganites in, e.g. next-generation capacitors and domain-wall nanoelectronics, or as catalysts or electrodes in fuel cells or electrolyzers. Furthermore, our approach is transferrable to other transition metal oxides, providing general guidelines for controlling their semiconducting properties.