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Title: Unraveling the Semiconducting/Metallic Discrepancy in Ni 3(HITP) 2

Here, Ni 3(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 Ni 3(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.
Authors:
ORCiD logo [1] ;  [2] ;  [1] ; ORCiD logo [1]
  1. Sandia National Lab. (SNL-CA), Livermore, CA (United States)
  2. Drexel Univ., Philadelphia, PA (United States)
Publication Date:
Report Number(s):
SAND-2017-12553J
Journal ID: ISSN 1948-7185; 658910; TRN: US1801534
Grant/Contract Number:
AC04-94AL85000
Type:
Accepted Manuscript
Journal Name:
Journal of Physical Chemistry Letters
Additional Journal Information:
Journal Volume: 9; Journal Issue: 3; Journal ID: ISSN 1948-7185
Publisher:
American Chemical Society
Research Org:
Sandia National Lab. (SNL-NM), Albuquerque, NM (United States)
Sponsoring Org:
USDOE National Nuclear Security Administration (NNSA)
Country of Publication:
United States
Language:
English
Subject:
36 MATERIALS SCIENCE
OSTI Identifier:
1421638

Foster, Michael E., Sohlberg, Karl, Allendorf, Mark D., and Talin, A. Alec. Unraveling the Semiconducting/Metallic Discrepancy in Ni3(HITP)2. United States: N. p., Web. doi:10.1021/acs.jpclett.7b03140.
Foster, Michael E., Sohlberg, Karl, Allendorf, Mark D., & Talin, A. Alec. Unraveling the Semiconducting/Metallic Discrepancy in Ni3(HITP)2. United States. doi:10.1021/acs.jpclett.7b03140.
Foster, Michael E., Sohlberg, Karl, Allendorf, Mark D., and Talin, A. Alec. 2018. "Unraveling the Semiconducting/Metallic Discrepancy in Ni3(HITP)2". United States. doi:10.1021/acs.jpclett.7b03140.
@article{osti_1421638,
title = {Unraveling the Semiconducting/Metallic Discrepancy in Ni3(HITP)2},
author = {Foster, Michael E. and Sohlberg, Karl and Allendorf, Mark D. and Talin, A. Alec},
abstractNote = {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.},
doi = {10.1021/acs.jpclett.7b03140},
journal = {Journal of Physical Chemistry Letters},
number = 3,
volume = 9,
place = {United States},
year = {2018},
month = {1}
}