Charge-transfer interface of insulating metal-organic frameworks with metallic conduction

Pooja Sindhu, K. S. Ananthram, Anil Jain, Kartick Tarafder and Nirmalya Ballav ()
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Pooja Sindhu: Indian Institute of Science Education and Research
K. S. Ananthram: National Institute of Technology Karnataka, Surathkal
Anil Jain: Bhabha Atomic Research Centre
Kartick Tarafder: National Institute of Technology Karnataka, Surathkal
Nirmalya Ballav: Indian Institute of Science Education and Research

Nature Communications, 2022, vol. 13, issue 1, 1-10

Abstract: Abstract Downsizing materials into hetero-structured thin film configurations is an important avenue to capture various interfacial phenomena. Metallic conduction at the interfaces of insulating transition metal oxides and organic molecules are notable examples, though, it remained elusive in the domain of coordination polymers including metal-organic frameworks (MOFs). MOFs are comprised of metal centers connected to organic linkers with an extended coordination geometry and potential void space. Poor orbitals overlap often makes these crystalline solids electrical insulators. Herein, we have fabricated hetero-structured thin film of a Mott and a band insulating MOFs via layer-by-layer method. Electrical transport measurements across the thin film evidenced an interfacial metallic conduction. The origin of such an unusual observation was understood by the first-principles density functional theory calculations; specifically, Bader charge analysis revealed significant accumulation and percolation of charge across the interface. We anticipate similar interfacial effects in other rationally designed hetero-structured thin films of MOFs.

Date: 2022
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DOI: 10.1038/s41467-022-35429-5

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