Revealing the Local Electronic Structure of a Single-Layer Covalent Organic Framework through Electronic Decoupling.

Daniel J Rizzo; Qingqing Dai; Christopher Bronner; Gregory Veber; Brian J Smith; Michio Matsumoto; Simil Thomas; Giang D Nguyen; Patrick R Forrester; William Zhao; Jakob H Jørgensen; William R. Dichtel; Felix R Fischer; Hong Li; Jean-Luc Bredas; Michael F. Crommie

doi:10.1021/acs.nanolett.9b03998

Revealing the Local Electronic Structure of a Single-Layer Covalent Organic Framework through Electronic Decoupling.

Daniel J Rizzo, Qingqing Dai, Christopher Bronner, Gregory Veber, Brian J Smith, Michio Matsumoto, Simil Thomas, Giang D Nguyen, Patrick R Forrester, William Zhao, Jakob H Jørgensen, William R. Dichtel, Felix R Fischer, Hong Li, Jean-Luc Bredas, Michael F. Crommie

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Abstract

Covalent organic frameworks (COFs) are molecule-based 2D and 3D materials that possess a wide range of mechanical and electronic properties. We have performed a joint experimental and theoretical study of the electronic structure of boroxine-linked COFs grown under ultrahigh vacuum conditions and characterized using scanning tunneling spectroscopy on Au(111) and hBN/Cu(111) substrates. Our results show that a single hBN layer electronically decouples the COF from the metallic substrate, thus suppressing substrate-induced broadening and revealing new features in the COF electronic local density of states (LDOS). The resulting sharpening of LDOS features allows us to experimentally determine the COF band gap, bandwidths, and the electronic hopping amplitude between adjacent COF bridge sites. These experimental parameters are consistent with the results of first-principles theoretical predictions.

Original language	English (US)
Journal	Nano letters
DOIs	https://doi.org/10.1021/acs.nanolett.9b03998
State	Published - Jan 15 2020

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10.1021/acs.nanolett.9b03998

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Rizzo, D. J., Dai, Q., Bronner, C., Veber, G., Smith, B. J., Matsumoto, M., Thomas, S., Nguyen, G. D., Forrester, P. R., Zhao, W., Jørgensen, J. H., Dichtel, W. R., Fischer, F. R., Li, H., Bredas, J.-L., & Crommie, M. F. (2020). Revealing the Local Electronic Structure of a Single-Layer Covalent Organic Framework through Electronic Decoupling. Nano letters. https://doi.org/10.1021/acs.nanolett.9b03998

@article{b685632cab3a44619c62ab0a8c0ad9a0,

title = "Revealing the Local Electronic Structure of a Single-Layer Covalent Organic Framework through Electronic Decoupling.",

abstract = "Covalent organic frameworks (COFs) are molecule-based 2D and 3D materials that possess a wide range of mechanical and electronic properties. We have performed a joint experimental and theoretical study of the electronic structure of boroxine-linked COFs grown under ultrahigh vacuum conditions and characterized using scanning tunneling spectroscopy on Au(111) and hBN/Cu(111) substrates. Our results show that a single hBN layer electronically decouples the COF from the metallic substrate, thus suppressing substrate-induced broadening and revealing new features in the COF electronic local density of states (LDOS). The resulting sharpening of LDOS features allows us to experimentally determine the COF band gap, bandwidths, and the electronic hopping amplitude between adjacent COF bridge sites. These experimental parameters are consistent with the results of first-principles theoretical predictions.",

author = "Rizzo, {Daniel J} and Qingqing Dai and Christopher Bronner and Gregory Veber and Smith, {Brian J} and Michio Matsumoto and Simil Thomas and Nguyen, {Giang D} and Forrester, {Patrick R} and William Zhao and J{\o}rgensen, {Jakob H} and Dichtel, {William R.} and Fischer, {Felix R} and Hong Li and Jean-Luc Bredas and Crommie, {Michael F.}",

note = "KAUST Repository Item: Exported on 2020-10-01 Acknowledgements: This research was supported by the Army Research Office Multidisciplinary University Research Initiative (MURI) program under Grant No. W911NF-15-1-0447 (STM spectroscopy, DFT analysis) and by the U.S. Department of Energy, Office of Basic Energy Sciences Nanomachine Program, under Contract No. DEAC02-05CH11231 (sample preparation). The work at Georgia Tech was supported in part by a grant of computer time from the DOD High Performance Computing Modernization Program.",

year = "2020",

month = jan,

day = "15",

doi = "10.1021/acs.nanolett.9b03998",

language = "English (US)",

journal = "Nano letters",

issn = "1530-6984",

publisher = "American Chemical Society",

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Rizzo, DJ, Dai, Q, Bronner, C, Veber, G, Smith, BJ, Matsumoto, M, Thomas, S, Nguyen, GD, Forrester, PR, Zhao, W, Jørgensen, JH, Dichtel, WR, Fischer, FR, Li, H, Bredas, J-L & Crommie, MF 2020, 'Revealing the Local Electronic Structure of a Single-Layer Covalent Organic Framework through Electronic Decoupling.', Nano letters. https://doi.org/10.1021/acs.nanolett.9b03998

TY - JOUR

T1 - Revealing the Local Electronic Structure of a Single-Layer Covalent Organic Framework through Electronic Decoupling.

AU - Rizzo, Daniel J

AU - Dai, Qingqing

AU - Bronner, Christopher

AU - Veber, Gregory

AU - Smith, Brian J

AU - Matsumoto, Michio

AU - Thomas, Simil

AU - Nguyen, Giang D

AU - Forrester, Patrick R

AU - Zhao, William

AU - Jørgensen, Jakob H

AU - Dichtel, William R.

AU - Fischer, Felix R

AU - Li, Hong

AU - Bredas, Jean-Luc

AU - Crommie, Michael F.

N1 - KAUST Repository Item: Exported on 2020-10-01 Acknowledgements: This research was supported by the Army Research Office Multidisciplinary University Research Initiative (MURI) program under Grant No. W911NF-15-1-0447 (STM spectroscopy, DFT analysis) and by the U.S. Department of Energy, Office of Basic Energy Sciences Nanomachine Program, under Contract No. DEAC02-05CH11231 (sample preparation). The work at Georgia Tech was supported in part by a grant of computer time from the DOD High Performance Computing Modernization Program.

PY - 2020/1/15

Y1 - 2020/1/15

N2 - Covalent organic frameworks (COFs) are molecule-based 2D and 3D materials that possess a wide range of mechanical and electronic properties. We have performed a joint experimental and theoretical study of the electronic structure of boroxine-linked COFs grown under ultrahigh vacuum conditions and characterized using scanning tunneling spectroscopy on Au(111) and hBN/Cu(111) substrates. Our results show that a single hBN layer electronically decouples the COF from the metallic substrate, thus suppressing substrate-induced broadening and revealing new features in the COF electronic local density of states (LDOS). The resulting sharpening of LDOS features allows us to experimentally determine the COF band gap, bandwidths, and the electronic hopping amplitude between adjacent COF bridge sites. These experimental parameters are consistent with the results of first-principles theoretical predictions.

AB - Covalent organic frameworks (COFs) are molecule-based 2D and 3D materials that possess a wide range of mechanical and electronic properties. We have performed a joint experimental and theoretical study of the electronic structure of boroxine-linked COFs grown under ultrahigh vacuum conditions and characterized using scanning tunneling spectroscopy on Au(111) and hBN/Cu(111) substrates. Our results show that a single hBN layer electronically decouples the COF from the metallic substrate, thus suppressing substrate-induced broadening and revealing new features in the COF electronic local density of states (LDOS). The resulting sharpening of LDOS features allows us to experimentally determine the COF band gap, bandwidths, and the electronic hopping amplitude between adjacent COF bridge sites. These experimental parameters are consistent with the results of first-principles theoretical predictions.

UR - http://hdl.handle.net/10754/661074

UR - https://pubs.acs.org/doi/10.1021/acs.nanolett.9b03998

UR - http://www.scopus.com/inward/record.url?scp=85078532436&partnerID=8YFLogxK

U2 - 10.1021/acs.nanolett.9b03998

DO - 10.1021/acs.nanolett.9b03998

M3 - Article

C2 - 31910625

SN - 1530-6984

JO - Nano letters

JF - Nano letters

ER -

Revealing the Local Electronic Structure of a Single-Layer Covalent Organic Framework through Electronic Decoupling.

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