SPINteger – Molecular-based interfaces supporting integer SPIN transfer.

在以信息技术为基础的当代社会，创造具有非凡性能的电子设备，以可以忽略不计的功耗每秒执行数十亿次逻辑运算，已经成为当务之急。为了维持这一技术的发展，除了硅基半导体之外，还需要新的材料，从这个角度来看，π共轭有机薄膜是取代无机半导体的最合适的候选材料之一。在这种情况下，新的分子多spinterface可以被设计成在低维系统中实现多功能性，为设计能够利用分子自旋态存储量子信息的设备提供了一种方法。近年来，研究表明介电层引起的功函数（WF）的巨大变化可以改变分子吸附物的电子能级排列，促进电荷通过隧道转移。由于缺乏杂化而阻碍了分数电荷转移，因此预计只有整数电荷转移是可能的。虽然这已经通过使用一种典型的介电材料实现了，比如超薄氧化镁（MgO）薄膜，外延生长在银（100）表面，SPINteger的目标是将这种方法扩展到一个真正的spinterface，该spinterface以三层结构实现，由铁衬底通过MgO薄层磁耦合到分子系统。SPINteger的主要目的是表征和控制这种支持自旋极化整数界面电荷转移的新型Fe/MgO/M分子多spinterface中的电子和空穴动力学。为此，将采用最先进的多学科方法，结合基于同步加速器的技术和飞秒XUV光源。特别是，结合角度分辨光发射光谱和密度泛函理论计算提供了最先进的能带结构表征方法之一：光发射层析成像（PT）。我们将把PT扩展到自旋和时间域，通过在同步加速器和fs-XUV辐射的大动量空间区域进行自旋分辨实验，获得占据和未占据分子状态及其动态的信息。整数电荷转移意味着创建定义良好的分子自旋态作为信息量子的可能性，为基于磁耦合单分子自旋的数据存储、量子计算和磁传感应用的新概念的发展开辟了道路。

Creating electronic devices with extraordinary performances, capable of performing billions of logical operations every second with a negligible power consumption has become an imperative in our contemporary society, which is based on information technology. To sustain this technological development, novel materials, beyond silicon-based semiconductors, will be needed and, in this perspective, π-conjugated organic films are one of the most suitable candidates to replace inorganic semiconductors. In this context, novel molecular multi-spinterfaces could be engineered to achieve multifunctionality in a low-dimensional system, offering a way to engineer devices capable of storing quantum information using the molecular spin state. Recently, it has been shown that the large changes in work function (WF) induced by a dielectric layer can modify the electron energy level alignment for molecular adsorbates, promoting charge transfer via tunneling. Since the fractional charge transfer is hindered due to the lack of hybridization, only integer charge transfer is expected to be possible. While this has already been achieved by employing a prototypical dielectric material, such as an ultrathin magnesium oxide (MgO) film, epitaxially grown on the silver (100) surface, SPINteger aims to extend this approach to a truly spinterfaces implemented in tri-layer configuration consisting of an iron substrate magnetically coupled to a molecular system through a MgO thin layer. The main goal of SPINteger is to characterize and control the electron and hole dynamics in this novel Fe/MgO/M molecular multi-spinterfaces supporting spin-polarized integer interface charge transfer. To this end, a state-of-the-art multidisciplinary approach combining synchrotron-based techniques and femtosecond XUV light sources will be used. In particular, combining angle-resolved photoemission spectroscopy and density functional theory calculations provides one of the most advanced methods for band structure characterization: photoemission tomography (PT). We will extend PT to the spin and time domains, by performing spin-resolved experiments in large momentum space regions with both synchrotron and fs-XUV radiation, gaining information on the occupied and unoccupied molecular states, as well as their dynamic. Integer charge transfer implies the possibility to create well-defined molecular spin state as a quantum of information opening the way to the development of novel concepts for data storage, quantum computing and magnetic sensing applications based on magnetically coupled single molecular spins.