Unraveling the Semiconducting/Metallic Discrepancy in Ni3(HITP)2

Foster, Michael E.; Sohlberg, Karl; Allendorf, Mark D.; Talin, A. Alec

doi:10.1021/acs.jpclett.7b03140

Title: Unraveling the Semiconducting/Metallic Discrepancy in Ni₃(HITP)₂

Journal Article · Wed Jan 10 00:00:00 EST 2018 · Journal of Physical Chemistry Letters

DOI:https://doi.org/10.1021/acs.jpclett.7b03140· OSTI ID:1421638

^[1]; Sohlberg, Karl ^[2]; Allendorf, Mark D. ^[1];

^[1]

Sandia National Lab. (SNL-CA), Livermore, CA (United States)
Drexel Univ., Philadelphia, PA (United States)

Here, Ni₃(2,3,6,7,10,11-hexaiminotriphenylene)₂ is a π-stacked layered metal–organic framework material with extended π-conjugation that is analogous to graphene. Published experimental results indicate that the material is semiconducting, but all theoretical studies to date predict the bulk material to be metallic. Given that previous experimental work was carried out on specimens containing complex nanocrystalline microstructures and the tendency for internal interfaces to introduce transport barriers, we apply DFT to investigate the influence of internal interface defects on the electronic structure of Ni₃(HITP)₂. The results show that interface defects can introduce a transport barrier by breaking the π-conjugation and/or decreasing the dispersion of the electronic bands near the Fermi level. We demonstrate that the presence of defects can open a small gap, in the range of 15–200 meV, which is consistent with the experimentally inferred hopping barrier.

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Research Organization:: Sandia National Lab. (SNL-NM), Albuquerque, NM (United States)

Sponsoring Organization:: USDOE National Nuclear Security Administration (NNSA)

Grant/Contract Number:: AC04-94AL85000

OSTI ID:: 1421638

Report Number(s):: SAND-2017-12553J; 658910; TRN: US1801534

Journal Information:: Journal of Physical Chemistry Letters, Vol. 9, Issue 3; ISSN 1948-7185

Publisher:: American Chemical SocietyCopyright Statement

Country of Publication:: United States

Language:: English

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Cited by: 63 works

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