Aeschlimann Raphaël, Preziosi Daniele, Scheiderer Philipp, Sing Michael, Valencia Sergio, Santamaria Jacobo, Luo Chen, Ryll Hanjo, Radu Florin, Claessen Ralph, Piamonteze Cinthia, Bibes Manuel
Unité Mixte de Physique, CNRS, Thales, Université Paris-Saclay, 91767, Palaiseau, France.
Physikalisches Institut and Röntgen Center for Complex Material Systems (RCCM), Universität Würzburg, Am Hubland, D-97074, Würzburg, Germany.
Adv Mater. 2018 May 30:e1707489. doi: 10.1002/adma.201707489.
When ferromagnetic films become ultrathin, key properties such as the Curie temperature and the saturation magnetization are usually depressed. This effect is thoroughly investigated in magnetic oxides such as half-metallic manganites, but much less in ferrimagnetic insulating perovskites such as rare-earth titanates RTiO , despite their appeal to design correlated 2D electron gases. Here, the magnetic properties of epitaxial DyTiO thin films are reported. While films thicker than about 50 nm show a bulk-like response, at low thickness a surprising increase of the saturation magnetization is observed. This behavior is described using a classical model of a "dead layer" but assuming that this layer is actually "living," that is, it responds to the magnetic field with a strong paramagnetic susceptibility. Through depth-dependent X-ray absorption and photoemission spectroscopy, it is shown that the "living-dead layer" corresponds to surface regions where magnetic (S = 1/2) Ti ions are replaced by nonmagnetic Ti ions. Hysteresis cycles at the Dy M and Ti L edges indicate that the surface Ti ions decouple the Dy ions, thus unleashing their strong paramagnetic response. Finally, it is shown how capping the DyTiO film can help increase the Ti content near the surface and thus recover a better ferrimagnetic behavior.
当铁磁薄膜变得超薄时,诸如居里温度和饱和磁化强度等关键特性通常会降低。这种效应在诸如半金属锰氧化物等磁性氧化物中得到了充分研究,但在诸如稀土钛酸盐RTiO₃等亚铁磁绝缘钙钛矿中研究较少,尽管它们对设计相关二维电子气很有吸引力。在此,报道了外延DyTiO₃薄膜的磁性。当薄膜厚度大于约50nm时表现出类似体材料的响应,而在低厚度时观察到饱和磁化强度惊人地增加。这种行为用“死层”的经典模型来描述,但假设该层实际上是“活的”,也就是说,它以强顺磁磁化率响应磁场。通过深度依赖的X射线吸收和光电子能谱表明,“活-死层”对应于磁性(S = 1/2)Ti离子被非磁性Ti离子取代的表面区域。Dy M边和Ti L边处的磁滞回线表明表面Ti离子使Dy离子解耦,从而释放出它们强烈的顺磁响应。最后,展示了如何通过覆盖DyTiO₃薄膜有助于增加表面附近的Ti含量,从而恢复更好的亚铁磁行为。