Jetnipat Songkerdthong, Thanasee Thanasarnsurapong, Adisak Boonchun, David J. Harding, Pichaya Pattanasattayavong
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引用次数: 0
Abstract
Copper(I) thiocyanate (CuSCN) has emerged as an excellent hole-transporting semiconductor with applications spanning across electronic and optoelectronic fields. The coordination chemistry of CuSCN allows for extensive structural versatility via ligand modification. In this work, we have developed a synthetic method that reliably produces phase pure [Cu(SCN)(3-XPy)]n complexes (Py = pyridyl; X = OMe, H, Br, and Cl) in a 1:1:1 ratio to yield two-dimensional (2D) structures with a Cu-SCN network. The single crystal structure of [Cu(SCN)(3-OMePy)]n is also reported herein. Complexes with X = OMe and H show similar structures, in which the 2D layers are analogous to the buckled 2D sheets of silicene or blue phosphorene. On the other hand, for complexes with X = Br and Cl, their rippled 2D structures resemble the puckered 2D sheets found in black phosphorene. The variation of the electron-withdrawing ability of the substituent group is found to systematically shift the electronic energy levels and band gaps of the complexes, allowing the 2D CuSCN-based materials to display optical absorptions and emissions in the visible range. In addition, first-principles calculations reveal that the drastic change in the electronic levels is a result of the emergence of the Py ligand electronic states below the SCN states. This work demonstrates that the structural, electronic, and optical properties of 2D Cu-SCN networks can be systematically tailored through ligand modification.
期刊介绍:
Molecular Systems Design & Engineering provides a hub for cutting-edge research into how understanding of molecular properties, behaviour and interactions can be used to design and assemble better materials, systems, and processes to achieve specific functions. These may have applications of technological significance and help address global challenges.