Key Laboratory of Optoelectronic Technology and Systems (Ministry of Education), College of Optoelectronic Engineering, Chongqing University, Chongqing 400044, China.
Department of Applied Physics, College of Physics, Chongqing University, Chongqing 401331, China.
J Chem Phys. 2018 Jul 14;149(2):024702. doi: 10.1063/1.5038655.
On the basis of first-principles calculations, we investigated the structural and electronic properties of the two-dimensional (2D) Au-1,3,5 triethynylbenzene (Au-TEB) framework, which has been recently synthesized by homocoupling reactions in experiments. Featured by the C-Au-C linkage, the 2D Au-TEB network has a kagome lattice by Au atoms and a hexagonal lattice by organic molecules within the same metal-organic framework (MOF), which exhibits intrinsic half-metallicity with one spin channel metallic and the other spin channel fully insulating with a large energy gap of 2.8 eV. Two branches of kagome bands are located near the Fermi level, with each branch including one flat band and two Dirac bands, which originates from the out-of-plane d and d orbitals of Au and may lead to many exotic topological quantum phases. We further studied the adsorption of F atoms, Cl atoms, and small gas molecules including O, CO, NO, and NH on the Au-TEB network, aiming to exploit its potential applications in gas sensors. Detailed analyses on adsorption geometry, energy, molecular orbital interaction, and electronic structure modification suggest the great potential of Au-TEP as a promising alternative for gas sensing. We expect these results to expand the universe of low-dimensional half-metallic MOF structures and shed new light on their practical applications in nanoelectronics/spintronics.
基于第一性原理计算，我们研究了二维（2D）Au-1,3,5-三乙炔苯（Au-TEB）骨架的结构和电子性质，该骨架最近通过实验中的同偶联反应合成。二维 Au-TEB 网络的特点是 C-Au-C 键合，由 Au 原子形成 kagome 晶格，由有机分子形成同一金属有机骨架（MOF）内的六方晶格，具有内在的半金属性，一个自旋通道为金属，另一个自旋通道完全绝缘，能隙为 2.8eV。两个 kagome 能带分支位于费米能级附近，每个分支包括一个扁平带和两个狄拉克带，这源于 Au 的面外 d 和 d 轨道，可能导致许多奇异拓扑量子相。我们进一步研究了 F 原子、Cl 原子和包括 O、CO、NO 和 NH 在内的小分子气体在 Au-TEB 网络上的吸附，旨在探索其在气体传感器中的潜在应用。对吸附几何形状、能量、分子轨道相互作用和电子结构修饰的详细分析表明，Au-TEP 作为气体传感器的一种很有前途的替代品具有很大的潜力。我们希望这些结果能够扩展低维半金属 MOF 结构的范围，并为它们在纳米电子学/自旋电子学中的实际应用提供新的思路。
