论文标题

白光产生分子材料:无定形/晶体结构与非线性光学特性之间的相关性

White-light generating molecular materials: correlation between the amorphous/crystalline structure and nonlinear optical properties

论文作者

Haust, Johannes, Belz, Jürgen, Müller, Marius, Klee, Benjamin Danilo, Vasco, Jonathan Link, Hüppe, Franziska, Léon, Irán Rojas, Christmann, Jan, Beyer, Andreas, Dehnen, Stefanie, Rosemann, Nils W., Pilgrim, Wolf-Christian, Chatterjee, Sangam, Volz, Kerstin

论文摘要

无定形材料是当今技术不可或缺的一部分,它们通常在整合中具有性能和多功能性。因此,未来的应用越来越旨在收获无定形状态的潜力。但是,使用基于衍射的技术来建立其结构 - 秘密关系本质上是具有挑战性的,但对于发展高级功能是极为理想的。在本文中,我们介绍了一组基于透射电子显微镜的技术,以局部量化材料的结构。这种独特的方法允许清楚地识别无定形和晶体区域的空间分布,并量化代表性模型系统的无定形区域的原子布置。我们研究了明确,官能化的阿甘坦型群集分子的合奏,该集群表现出异常有希望的非线性光学特性的不清楚起源。三种模型化合物的纳米结构([[(PHSN)4S6],[(NPSN)4S6],[(CPSN)4S6])与它们的特征光学响应相关。这些结果突出了当了解微观起源时,无定形分子材料的优势性能。

Amorphous materials are integral part of todays technology, they commonly are performant and versatile in integration. Consequently, future applications increasingly aim to harvest the potential of the amorphous state. Establishing its structure-property relationship, however, is inherently challenging using diffraction-based techniques yet is extremely desirable for developing advanced functionalities. In this article, we introduce a set of transmission electron microscopy-based techniques to locally quantify the structure of a material. This unique approach allows to clearly identify the spatial distribution of amorphous and crystalline regions and to quantify atomic arrangements of amorphous regions of a representative model system. We study an ensemble of well-defined, functionalized adamantane-type cluster molecules exhibiting exceptionally promising nonlinear optical properties of unclear origin. The nanoscopic structure for three model compounds ([(PhSn)4S6], [(NpSn)4S6], [(CpSn)4S6]) correlates with their characteristic optical responses. These results highlight the advantageous properties of amorphous molecular materials when understanding the microscopic origin.

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