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首页> 外文期刊>The journal of physical chemistry, C. Nanomaterials and interfaces >Thermodynamics of the Segregation of a Kinetically Trapped Two-Dimensional Amorphous Metal-Organic Network
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Thermodynamics of the Segregation of a Kinetically Trapped Two-Dimensional Amorphous Metal-Organic Network

机译：动力学捕获的二维非晶态金属-有机网络的分离热力学。

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摘要

Surface-confined self-assembled molecular networks are commonly described as crystalline structures with short- and long-range order. Few exceptions to this trend are found in the literature reporting on amorphous and glassy networks and, discussing the origins of their disordered nature at the atomic, scale. Here, we show that an amorphous two component metal-organic network can be synthesized on a crystalline metal surface at room temperature by vapor deposition of organic molecules and metal atoms. Scanning tunneling microscopy reveals the transformation of a crystalline close packed organic layer into a disordered porous layer formed through the self-assembly of an organic semiconductor functionalized with two cyano groups upon introduction of iron atoms on Ag(111). In contrast to the commonly observed preference for trigonal crystal symmetry in 2D systems that form, glassy networks, our metal organic network favors rhombic or square tessellation of the surface. Statistical analysis of the network's morphology reveals that entropy plays a critical part in its stabilization. Phase segregation of the binary mixture of monodisperse metal atoms and organic molecules into spatially separate homogeneously crystalline domains of molecules and metal atoms upon thermal annealing and subsequent cooling is observed. This suggests that the amorphous network is kinetically trapped at room temperature during the preparation process.
机译：表面受限的自组装分子网络通常被描述为具有短程和长程顺序的晶体结构。关于非晶态和玻璃态网络的文献报道很少发现这种趋势的例外，并且在原子尺度上讨论了它们无序性的起源。在这里，我们表明可以通过有机分子和金属原子的气相沉积在室温下在晶体金属表面上合成非晶态的两组分金属-有机网络。扫描隧道显微镜显示，在Ag（111）上引入铁原子后，通过用两个氰基官能化的有机半导体的自组装，晶体紧密堆积的有机层转变为无序的多孔层。与通常在形成玻璃状网络的2D系统中偏爱三角晶体对称性相反，我们的金属有机网络偏爱表面的菱形或方形镶嵌。对网络形态的统计分析表明，熵在其稳定中起着至关重要的作用。在热退火和随后的冷却下，观察到单分散金属原子和有机分子的二元混合物的相分离成分子和金属原子的空间上分离的均匀结晶域。这表明在制备过程中，非晶态网络在室温下被动力学捕获。

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