Dichotomy between frustrated local spins and conjugated electrons in a two-dimensional metal–organic framework
Abstract
Dichotomy between local spins and conjugated electrons spawns various exotic physical phenomena, however, it has mostly been reported in three-dimensional (3D) inorganic systems. We demonstrate, for the first time, that a rare 2D metal–organic framework exhibits intriguing dichotomy behavior, which can be directly identified through scanning tunneling microscopy/spectroscopy (STM/STS). In a newly synthesized Cu-hexaiminobenzene [Cu3(HAB)2], on the one hand, the Cu2+ ions form an ideal S–1/2 antiferromagnetic (AFM) kagome lattice; on the other hand, the conjugated-electrons from the organic ligands produce a frustrated πx,y model on a honeycomb lattice, giving rise to completely dispersionless energy bands around the Fermi level that favour the ferromagnetic (FM) state. Remarkably, the frustrated local spins and conjugated electrons interact through a strong FM Hund's coupling, giving rise to a wide range of intriguing quantum phases. Furthermore, we propose that this dichotomy can be directly characterized through STM/STS measurements due to its special 2D nature, which provides a unique exciting platform to investigate the dichotomy of frustrated spins and electrons in a single lattice.
- Authors:
-
- Univ. of Utah, Salt Lake City, UT (United States); Univ. of Minnesota, Minneapolis, MN (United States)
- Tsinghua Univ., Beijing (China)
- Southern Univ. of Science and Technology, Shenzhen (China)
- Shandong Univ., Jinan (China)
- Univ. of Utah, Salt Lake City, UT (United States)
- Publication Date:
- Research Org.:
- Lawrence Berkeley National Laboratory (LBNL), Berkeley, CA (United States). National Energy Research Scientific Computing Center (NERSC); Univ. of Utah, Salt Lake City, UT (United States)
- Sponsoring Org.:
- USDOE Office of Science (SC), Basic Energy Sciences (BES); National Science Foundation (NSF); National Natural Science Foundation of China (NSFC)
- OSTI Identifier:
- 1543815
- Alternate Identifier(s):
- OSTI ID: 1487170
- Grant/Contract Number:
- FG02-04ER46148; DMR-1121252; 11774196
- Resource Type:
- Accepted Manuscript
- Journal Name:
- Nanoscale
- Additional Journal Information:
- Journal Volume: 11; Journal Issue: 3; Journal ID: ISSN 2040-3364
- Publisher:
- Royal Society of Chemistry
- Country of Publication:
- United States
- Language:
- English
- Subject:
- 42 ENGINEERING; Chemistry; Science & Technology - Other Topics; Materials Science; Physics
Citation Formats
Jiang, Wei, Liu, Zheng, Mei, Jia-Wei, Cui, Bin, and Liu, Feng. Dichotomy between frustrated local spins and conjugated electrons in a two-dimensional metal–organic framework. United States: N. p., 2018.
Web. doi:10.1039/c8nr08479c.
Jiang, Wei, Liu, Zheng, Mei, Jia-Wei, Cui, Bin, & Liu, Feng. Dichotomy between frustrated local spins and conjugated electrons in a two-dimensional metal–organic framework. United States. https://doi.org/10.1039/c8nr08479c
Jiang, Wei, Liu, Zheng, Mei, Jia-Wei, Cui, Bin, and Liu, Feng. Fri .
"Dichotomy between frustrated local spins and conjugated electrons in a two-dimensional metal–organic framework". United States. https://doi.org/10.1039/c8nr08479c. https://www.osti.gov/servlets/purl/1543815.
@article{osti_1543815,
title = {Dichotomy between frustrated local spins and conjugated electrons in a two-dimensional metal–organic framework},
author = {Jiang, Wei and Liu, Zheng and Mei, Jia-Wei and Cui, Bin and Liu, Feng},
abstractNote = {Dichotomy between local spins and conjugated electrons spawns various exotic physical phenomena, however, it has mostly been reported in three-dimensional (3D) inorganic systems. We demonstrate, for the first time, that a rare 2D metal–organic framework exhibits intriguing dichotomy behavior, which can be directly identified through scanning tunneling microscopy/spectroscopy (STM/STS). In a newly synthesized Cu-hexaiminobenzene [Cu3(HAB)2], on the one hand, the Cu2+ ions form an ideal S–1/2 antiferromagnetic (AFM) kagome lattice; on the other hand, the conjugated-electrons from the organic ligands produce a frustrated πx,y model on a honeycomb lattice, giving rise to completely dispersionless energy bands around the Fermi level that favour the ferromagnetic (FM) state. Remarkably, the frustrated local spins and conjugated electrons interact through a strong FM Hund's coupling, giving rise to a wide range of intriguing quantum phases. Furthermore, we propose that this dichotomy can be directly characterized through STM/STS measurements due to its special 2D nature, which provides a unique exciting platform to investigate the dichotomy of frustrated spins and electrons in a single lattice.},
doi = {10.1039/c8nr08479c},
journal = {Nanoscale},
number = 3,
volume = 11,
place = {United States},
year = {Fri Nov 23 00:00:00 EST 2018},
month = {Fri Nov 23 00:00:00 EST 2018}
}
Web of Science
Works referenced in this record:
Redox Control and High Conductivity of Nickel Bis(dithiolene) Complex π-Nanosheet: A Potential Organic Two-Dimensional Topological Insulator
journal, October 2014
- Kambe, Tetsuya; Sakamoto, Ryota; Kusamoto, Tetsuro
- Journal of the American Chemical Society, Vol. 136, Issue 41
Template-directed supramolecular self-assembly of coordination dumbbells at surfaces
journal, January 2007
- Lin, Nian; Langner, Alexander; Tait, Steven L.
- Chemical Communications, Issue 46
Redox chemistry and spectroscopy of toluene-3,4-dithiol (TDTH2) and of its M(TDT)22-/- complexes with zinc(II), copper(II), nickel(II), cobalt(II), iron(II), and manganese(II). Formation of a stable dn-(.cntdot.SR) bond upon oxidation by one electron
journal, March 1986
- Sawyer, Donald T.; Srivatsa, G. Susan.; Bodini, Mario E.
- Journal of the American Chemical Society, Vol. 108, Issue 5
Tuning interfacial spin filters from metallic to resistive within a single organic semiconductor family
journal, June 2017
- Wang, Jingying; Deloach, Andrew; Jiang, Wei
- Physical Review B, Vol. 95, Issue 24
Metal–organic framework materials as catalysts
journal, January 2009
- Lee, JeongYong; Farha, Omar K.; Roberts, John
- Chemical Society Reviews, Vol. 38, Issue 5, p. 1450-1459
Prediction of large gap flat Chern band in a two-dimensional metal-organic framework
journal, January 2018
- Su, Ninghai; Jiang, Wei; Wang, Zhengfei
- Applied Physics Letters, Vol. 112, Issue 3
First-principles design of a half-filled flat band of the kagome lattice in two-dimensional metal-organic frameworks
journal, August 2016
- Yamada, Masahiko G.; Soejima, Tomohiro; Tsuji, Naoto
- Physical Review B, Vol. 94, Issue 8
High Electrical Conductivity in Ni 3 (2,3,6,7,10,11-hexaiminotriphenylene) 2 , a Semiconducting Metal–Organic Graphene Analogue
journal, April 2014
- Sheberla, Dennis; Sun, Lei; Blood-Forsythe, Martin A.
- Journal of the American Chemical Society, Vol. 136, Issue 25
Hydrogen storage in metal–organic frameworks
journal, January 2009
- Murray, Leslie J.; Dincă, Mircea; Long, Jeffrey R.
- Chemical Society Reviews, Vol. 38, Issue 5, p. 1294-1314
Oxidation-promoted Interfacial Synthesis of Redox-active Bis(diimino)nickel Nanosheet
journal, February 2018
- Phua, Eunice J. H.; Wu, Kuo-Hui; Wada, Keisuke
- Chemistry Letters, Vol. 47, Issue 2
CMR manganites: physics, thin films and devices
journal, April 2003
- Haghiri-Gosnet, A-M; Renard, J-P
- Journal of Physics D: Applied Physics, Vol. 36, Issue 8
Introduction to Metal–Organic Frameworks
journal, September 2011
- Zhou, Hong-Cai; Long, Jeffrey R.; Yaghi, Omar M.
- Chemical Reviews, Vol. 112, Issue 2, p. 673-674
Hexaaminobenzene as a building block for a Family of 2D Coordination Polymers
journal, December 2016
- Lahiri, Nabajit; Lotfizadeh, Neda; Tsuchikawa, Ryuichi
- Journal of the American Chemical Society, Vol. 139, Issue 1
Stability of the Spontaneous Quantum Hall State in the Triangular Kondo-Lattice Model
journal, December 2010
- Kato, Yasuyuki; Martin, Ivar; Batista, C. D.
- Physical Review Letters, Vol. 105, Issue 26
Insulator-metal transition and giant magnetoresistance in
journal, May 1995
- Urushibara, A.; Moritomo, Y.; Arima, T.
- Physical Review B, Vol. 51, Issue 20
Resistance Minimum in Dilute Magnetic Alloys
journal, July 1964
- Kondo, J.
- Progress of Theoretical Physics, Vol. 32, Issue 1, p. 37-49
Selective gas adsorption and separation in metal–organic frameworks
journal, January 2009
- Li, Jian-Rong; Kuppler, Ryan J.; Zhou, Hong-Cai
- Chemical Society Reviews, Vol. 38, Issue 5, p. 1477-1504
Beyond post-synthesis modification: evolution of metal–organic frameworks via building block replacement
journal, January 2014
- Deria, Pravas; Mondloch, Joseph E.; Karagiaridi, Olga
- Chem. Soc. Rev., Vol. 43, Issue 16
Spin-polarized scanning tunnelling microscopy
journal, March 2003
- Bode, M.
- Reports on Progress in Physics, Vol. 66, Issue 4
Current-Induced Magnetization Switching with a Spin-Polarized Scanning Tunneling Microscope
journal, September 2007
- Krause, S.; Berbil-Bautista, L.; Herzog, G.
- Science, Vol. 317, Issue 5844
Iron pnictides as a new setting for quantum criticality
journal, March 2009
- Dai, J.; Si, Q.; Zhu, J. -X.
- Proceedings of the National Academy of Sciences, Vol. 106, Issue 11
Li doped kagome spin liquid compounds
journal, January 2018
- Jiang, Wei; Huang, Huaqing; Mei, Jia-Wei
- Physical Chemistry Chemical Physics, Vol. 20, Issue 33
Assembling Isostructural Metal-Organic Coordination Architectures on Cu(100), Ag(100) and Ag(111) Substrates
journal, December 2008
- Tait, Steven L.; Langner, Alexander; Lin, Nian
- ChemPhysChem, Vol. 9, Issue 17
π-Conjugated Nickel Bis(dithiolene) Complex Nanosheet
journal, February 2013
- Kambe, Tetsuya; Sakamoto, Ryota; Hoshiko, Ken
- Journal of the American Chemical Society, Vol. 135, Issue 7
Prediction of two-dimensional nodal-line semimetals in a carbon nitride covalent network
journal, January 2018
- Chen, Haiyuan; Zhang, Shunhong; Jiang, Wei
- Journal of Materials Chemistry A, Vol. 6, Issue 24
Intrinsic quantum anomalous hall effect in a two-dimensional anilato-based lattice
journal, January 2018
- Ni, Xiaojuan; Jiang, Wei; Huang, Huaqing
- Nanoscale, Vol. 10, Issue 25
Deconstructing the Crystal Structures of Metal–Organic Frameworks and Related Materials into Their Underlying Nets
journal, September 2011
- O’Keeffe, Michael; Yaghi, Omar M.
- Chemical Reviews, Vol. 112, Issue 2, p. 675-702
Electronic Structure of Bis( o -iminobenzosemiquinonato)metal Complexes (Cu, Ni, Pd). The Art of Establishing Physical Oxidation States in Transition-Metal Complexes Containing Radical Ligands
journal, March 2001
- Chaudhuri, Phalguni; Verani, Claudio Nazari; Bill, Eckhard
- Journal of the American Chemical Society, Vol. 123, Issue 10
High-throughput computational screening of metal–organic frameworks
journal, January 2014
- Colón, Yamil J.; Snurr, Randall Q.
- Chem. Soc. Rev., Vol. 43, Issue 16
Giant magnetoresistance of manganese oxides with a layered perovskite structure
journal, March 1996
- Moritomo, Y.; Asamitsu, A.; Kuwahara, H.
- Nature, Vol. 380, Issue 6570
Flat Chern Band in a Two-Dimensional Organometallic Framework
journal, March 2013
- Liu, Zheng; Wang, Zheng-Fei; Mei, Jia-Wei
- Physical Review Letters, Vol. 110, Issue 10
A Theory for a Self-Trapped Antiferromagnetic Polaron at T =0 K
journal, September 1972
- Umehara, Masakatu; Kasuya, Tadao
- Journal of the Physical Society of Japan, Vol. 33, Issue 3
Possible highT c superconductivity in the Ba?La?Cu?O system
journal, June 1986
- Bednorz, J. G.; M�ller, K. A.
- Zeitschrift f�r Physik B Condensed Matter, Vol. 64, Issue 2
Localized Magnetic States in Metals
journal, October 1961
- Anderson, P. W.
- Physical Review, Vol. 124, Issue 1
Role of conduction-electron – local-moment exchange in antiferromagnetic semiconductors: Ferrons and bound magnetic polarons
journal, June 1985
- Mauger, A.; Mills, D. L.
- Physical Review B, Vol. 31, Issue 12
Phase diagram of the Kondo lattice model on the kagome lattice
journal, January 2016
- Ghosh, Shivam; O'Brien, Patrick; Henley, Christopher L.
- Physical Review B, Vol. 93, Issue 2
Tailoring molecular layers at metal surfaces
journal, January 2010
- Bartels, Ludwig
- Nature Chemistry, Vol. 2, Issue 2
Luttinger-volume violating Fermi liquid in the pseudogap phase of the cuprate superconductors
journal, April 2012
- Mei, Jia-Wei; Kawasaki, Shinji; Zheng, Guo-Qing
- Physical Review B, Vol. 85, Issue 13
Cu 3 (hexaiminotriphenylene) 2 : An Electrically Conductive 2D Metal-Organic Framework for Chemiresistive Sensing
journal, February 2015
- Campbell, Michael G.; Sheberla, Dennis; Liu, Sophie F.
- Angewandte Chemie International Edition, Vol. 54, Issue 14
Giant Magnetoresistance and Related Properties of Rare-Earth Manganates and Other Oxide Systems
journal, January 1996
- Rao, C. N. R.; Cheetham, A. K.; Mahesh, R.
- Chemistry of Materials, Vol. 8, Issue 10
-Virtual-Bound-State Formation in Ce at Low Temperatures
journal, December 1975
- Andres, K.; Graebner, J. E.; Ott, H. R.
- Physical Review Letters, Vol. 35, Issue 26
Weak magnetism and non-Fermi liquids near heavy-fermion critical points
journal, January 2004
- Senthil, T.; Vojta, Matthias; Sachdev, Subir
- Physical Review B, Vol. 69, Issue 3
Polaron coherence condensation as the mechanism for colossal magnetoresistance in layered manganites
journal, December 2007
- Mannella, N.; Yang, W. L.; Tanaka, K.
- Physical Review B, Vol. 76, Issue 23
Two-Dimensional Band Structure in Honeycomb Metal–Organic Frameworks
journal, August 2018
- Kumar, Avijit; Banerjee, Kaustuv; Foster, Adam S.
- Nano Letters, Vol. 18, Issue 9
Hidden Multiple-Spin Interactions as an Origin of Spin Scalar Chiral Order in Frustrated Kondo Lattice Models
journal, February 2012
- Akagi, Yutaka; Udagawa, Masafumi; Motome, Yukitoshi
- Physical Review Letters, Vol. 108, Issue 9
Doping a Mott insulator: Physics of high-temperature superconductivity
journal, January 2006
- Lee, Patrick A.; Nagaosa, Naoto; Wen, Xiao-Gang
- Reviews of Modern Physics, Vol. 78, Issue 1
Cation exchange at the secondary building units of metal–organic frameworks
journal, January 2014
- Brozek, C. K.; Dincă, M.
- Chem. Soc. Rev., Vol. 43, Issue 16
Prediction of a Two-Dimensional Organic Topological Insulator
journal, May 2013
- Wang, Z. F.; Su, Ninghai; Liu, Feng
- Nano Letters, Vol. 13, Issue 6, p. 2842-2845
Signature of Metallic Behavior in the Metal–Organic Frameworks M 3 (hexaiminobenzene) 2 (M = Ni, Cu)
journal, September 2017
- Dou, Jin-Hu; Sun, Lei; Ge, Yicong
- Journal of the American Chemical Society, Vol. 139, Issue 39
EuTe. I. Magnetic Behavior of Insulating and Conducting Single Crystals
journal, April 1972
- Oliveira, N. F.; Foner, S.; Shapira, Y.
- Physical Review B, Vol. 5, Issue 7
Stability condition for the paramagnetic polaron in a magnetic semiconductor
journal, October 1970
- Kasuya, T.; Yanase, A.; Takeda, T.
- Solid State Communications, Vol. 8, Issue 19
Synthesis of Metal-Organic Frameworks (MOFs): Routes to Various MOF Topologies, Morphologies, and Composites
journal, September 2011
- Stock, Norbert; Biswas, Shyam
- Chemical Reviews, Vol. 112, Issue 2
Bis(aminothiolato)nickel nanosheet as a redox switch for conductivity and an electrocatalyst for the hydrogen evolution reaction
journal, January 2017
- Sun, Xinsen; Wu, Kuo-Hui; Sakamoto, Ryota
- Chemical Science, Vol. 8, Issue 12
Flat Bands and Wigner Crystallization in the Honeycomb Optical Lattice
journal, August 2007
- Wu, Congjun; Bergman, Doron; Balents, Leon
- Physical Review Letters, Vol. 99, Issue 7
Electronic Structure of Square Planar Bis(benzene-1,2-dithiolato)metal Complexes [M(L) 2 ] z ( z = 2−, 1−, 0; M = Ni, Pd, Pt, Cu, Au): An Experimental, Density Functional, and Correlated ab Initio Study
journal, July 2005
- Ray, Kallol; Weyhermüller, Thomas; Neese, Frank
- Inorganic Chemistry, Vol. 44, Issue 15
Theoretical Evidence for the Singlet Diradical Character of Square Planar Nickel Complexes Containing Two o -Semiquinonato Type Ligands
journal, August 2002
- Bachler, Vinzenz; Olbrich, Gottfried; Neese, Frank
- Inorganic Chemistry, Vol. 41, Issue 16
Cu 3 (hexaiminotriphenylene) 2 : An Electrically Conductive 2D Metal-Organic Framework for Chemiresistive Sensing
journal, February 2015
- Campbell, Michael G.; Sheberla, Dennis; Liu, Sophie F.
- Angewandte Chemie, Vol. 127, Issue 14
Polaron Coherence Condensation as the Mechanism for Colossal Magnetoresistance in Layered Manganites
text, January 2007
- Mannella, N.; Yang, W. L.; Tanaka, K.
- arXiv
Stability of spontaneous quantum Hall state in the Triangular Kondo-lattice model
text, January 2010
- Kato, Yasuyuki; Martin, Ivar; Batista, C. D.
- arXiv
Luttinger-volume violating Fermi liquid in the pseudogap phase of the cuprate superconductors
text, January 2011
- Mei, Jia-Wei; Kawasaki, Shinji; Zheng, Guo-Qing
- arXiv
Flat Chern Band in a Two-Dimensional Organometallic Framework
text, January 2012
- Liu, Zheng; Wang, Zheng-Fei; Mei, Jia-Wei
- arXiv
First-Principles Design of a Half-Filled Flat Band of the Kagome Lattice in Two-Dimensional Metal-Organic Frameworks
text, January 2015
- Yamada, Masahiko G.; Soejima, Tomohiro; Tsuji, Naoto
- arXiv
Weak magnetism and non-Fermi liquids near heavy-fermion critical points
text, January 2003
- Senthil, T.; Vojta, Matthias; Sachdev, Subir
- arXiv
Works referencing / citing this record:
The shielding effects of a C 60 cage on the magnetic moments of transition metal atoms inside the corner holes of Si(111)-(7 × 7)
journal, January 2019
- Shao, Xiji; Li, Lin; Shi, Xingqiang
- Nanoscale, Vol. 11, Issue 13
Flat bands and nontrivial topological properties in an extended Lieb lattice
journal, December 2019
- Bhattacharya, Ankita; Pal, Biplab
- Physical Review B, Vol. 100, Issue 23
Methods for the construction of interacting many-body Hamiltonians with compact localized states in geometrically frustrated clusters
journal, March 2020
- Santos, F. D. R.; Dias, R. G.
- Scientific Reports, Vol. 10, Issue 1