Proceedings of nanoGe Fall Meeting 2018 (NFM18)
DOI: https://doi.org/10.29363/nanoge.nfm.2018.043
Publication date: 6th July 2018
Metal-organic frameworks (MOFs) are coordination polymers consisting of metal ions connected by organic ligands. Besides the traditional applications in gas storage and separation as well as catalysis, the long-range crystalline order in MOFs and the tunable coupling between their organic and inorganic constituents have recently led to the design and synthesis of (semi-)conducting MOFs, opening the path for their application in opto-electronics. Yet, despite being a critical aspect for the development of MOF based electronics, the true nature of charge transport in MOFs, i.e. whether hopping or band-like transport occurs, has remained unresolved to date.
Here we report a time-resolved high-frequency (terahertz) conductivity study of a newly developed Fe3(THT)2 (THT=2,3,6,7,10,11-hexathioltriphenylene) two-dimensional MOF. The novel π-d conjugated samples, synthesized through interfacial method at room temperature, are obtained as a large-area, free-standing film with tunable geometry (size and thickness). The Fe3(THT)2 films are conductive (~1 S/cm), porous (specific surface area of 526±5 m2/g) and semiconducting (with a ~250 meV direct bandgap). We demonstrate for the first time band-like charge transport in MOFs. This finding is directly apparent from the Drude-type high-frequency (terahertz) photo-conductivity response obtained in the samples; revealing free-moving, delocalized charge carriers displaying ~200 cm2/Vs mobilities at room temperature; a record mobility for MOFs. The temperature dependence of the mobility reveals that the main scattering mechanism limiting the mobility and hence band-like charge transport in this material is related to impurity scattering, so that material improvements may further increase the mobility.
The demonstration of band-like charge transport in MOFs reveal the potential of (porous) conductive MOFs to be employed as active materials in opto-electronics devices.
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