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  1. Abstract

    The incorporation of metal-organic frameworks into advanced devices remains a desirable goal, but progress is hindered by difficulties in preparing large crystalline metal-organic framework films with suitable electronic performance. We demonstrate the direct growth of large-area, high quality, and phase pure single metal-organic framework crystals through chemical vapor deposition of a dimolybdenum paddlewheel precursor, Mo2(INA)4. These exceptionally uniform, high quality crystals cover areas up to 8600 µm2and can be grown down to thicknesses of 30 nm. Moreover, scanning tunneling microscopy indicates that the Mo2(INA)4clusters assemble into a two-dimensional, single-layer framework. Devices are readily fabricated from single vapor-phase grown crystals and exhibit reversible 8-fold changes in conductivity upon illumination at modest powers. Moreover, we identify vapor-induced single crystal transitions that are reversible and responsible for 30-fold changes in conductivity of the metal-organic framework as monitored by in situ device measurements. Gas-phase methods, including chemical vapor deposition, show broader promise for the preparation of high-quality molecular frameworks, and may enable their integration into devices, including detectors and actuators.

     
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  2. This review identifies how recent advances in controlling the structure and properties of MOF and COF thin films can be used to establish 2D molecular crystals as a new material platform with key applications in catalysis, sensing, separations, and electronics. In addition to summarizing research efforts surrounding the synthesis, characterization and utilization of 2D and thin film MOFs and COFs, this review identifies exigent challenges in their development, and motivates the search for new synthetic methods, advanced analytical techniques, and creative applications. Ultimately, 2D molecular lattices, be they 2D MOFs or COFs, are a compelling platform through which to discover new and emergent properties and to expand the library of 2D materials. 
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  3. A growing focus on the use of coordination polymers for active device applications motivates the search for candidate materials with integrated and optimized charge transport modes. We show herein the synthesis of a linear coordination polymer comprised of Mo 2 (INA) 4 (INA = isonicotinate) metal–organic clusters. Single-crystal X-ray structure determination shows that this cluster crystallizes into one-dimensional molecular chains, whose INA-linked Mo 2 cores engage in alternate axial and equatorial binding motifs along the chain axis. Electron paramagnetic resonance spectra, absorption spectra, and density functional theory calculations show that the aforementioned linear coordination environment significantly modifies the electronic structure of the clusters. This work expands the synthetic foundation for assembly of coordination polymers with tailorable dimensionalities and charge transport properties. 
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