Optimization of Cooperative Effects in Strongly Organized Molecular Assemblies for Organic Electronics Applications

在过去十年中，有机和分子电子学领域的进展在科学上是丰富的，在技术上是非常有前途的。在许多方面都取得了重大进展：建立具有卓越结构控制的超分子系统的方法，或以分子精度生长薄膜的方法，毫无疑问揭示表面和界面基本特征的光谱技术，以及性能不断提高的设备的持续生产。尽管取得了重大进展，但该领域仍然是最开放和最具挑战性的研究领域之一，计算建模的支持可用于指导和加速高性能电活性部件的生产。在需要解决的最重要的科学问题中，我们注意到(1)在2D和3D组装系统中分子间相互作用对其产生的电子、电气和结构特性的作用；(2)这些相互作用对组装系统促进和控制表面掺杂能力的重要性；最后(3)在原子尺度上定量描述分离和组装系统一旦吸附在表面上的分子间相互作用的性质和大小。为了解决这些悬而未决的问题，我们将使用最先进的DFT方法和扫描隧道显微镜（STM）模拟作为我们的主要计算技术来描述从孤立物种到模型表面上组装纳米结构的吸附特性的变化。在目前的提案中，我们希望扩大我们在电子结构计算方面的专业知识，包括使用和开发我们的STM工具来研究(i)大规模二维纳米结构，（ii）多层和三维（3D）组件，以及（iii）开发考虑分子弛豫的动态侵入式STM模拟器。我们还将继续目前在复杂和非均质系统中电荷渗透建模方面的研究工作，并将通过研究含有成分和结构缺陷的无机CIGS （Cu-In-Ga-Se）纳米线来扩展我们在光伏材料方面的专业知识。

The progress observed during the last decade in the field of organic and molecular electronics is scientifically rich and technologically very promising. Major advancement has been observed in many directions: approaches that allow to build supramolecular systems with excellent architectural control or to grow thin films with molecular precision, spectroscopic techniques that undoubtly reveal fundamental characteristics of surfaces and interfaces, and the continuous production of devices with improved performance. Despite a significant progress, this field remains one of the most open and challenging research areas where support from computational modeling can be used to guide and accelerate the production of high performance electroactive component. Among the most important scientific issues to address, we note (1) the role of intermolecular interaction within 2D and 3D assembled systems on their resulting electronic, electrical and structural properties, (2) the importance of these interactions on the capability of assembled systems to promote and control the doping of surfaces, and finally (3) to quantitatively describe the nature and magnitude of intermolecular interactions at the atomic scale for isolated and assembled systems once adsorbed on a surface. In order to address these open questions, we will use state-of-the-art DFT methods and scanning tunnelling microscopy (STM) simulations as our main computational techniques to describe the variation of adsorption properties from isolated species to assembled nanostructures on model surfaces. In the present proposal, we want to extent our expertise in electronic structure calculations including the use and development of our STM tools to investigate (i) large scale 2D nanostructures, (ii) multilayer and tridimensional (3D) assemblies, and (iii) to develop a dynamical intrusive STM simulator that considers molecular relaxation. We will also pursuit our present research efforts on the modeling of percolation of charges in complex and heterogeneous systems, and we will extent our expertise in photovoltaic materials by investigating inorganic CIGS (Cu-In-Ga-Se) nanowires containing composition and structural defects.