Highly Degenerate Ground States in a Frustrated Antiferromagnetic Kagome Lattice in a Two-Dimensional Metal–Organic Framework

Hua, Muqing; Xia, Bowen; Wang, Miao; Li, En; Liu, Jing; Wu, Ta‐You; Wang, Yifan; Li, Ruoning; Ding, Honghe; Hu, Jun; Wang, Yongfeng; Xu, Hu; Zhao, Wei; Lin, Nian

doi:10.1021/acs.jpclett.1c00598

Cited by 30 publications

(34 citation statements)

References 62 publications

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“…2D MOFs have been synthesized on metal surfaces by following the concepts of supramolecular coordination chemistry. , So far, most of the 2D MOFs are made on coinage metal surfaces, − where the interaction with the metal substrate strongly masks the intrinsic electronic properties of the MOF. This can be overcome by using weakly interacting substrates (such as graphene and hBN) that allow probing of the intrinsic exotic electronic properties of 2D MOFs. − However, to realize the exciting prospect of truly designer materials, it is important to demonstrate MOF synthesis on other 2D substrates.…”

Section: Introductionmentioning

confidence: 99%

Two-Dimensional Metal–Organic Framework on Superconducting NbSe₂

et al. 2021

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The combination of two-dimensional (2D) materials into vertical heterostructures has emerged as a promising path to designer quantum materials with exotic properties. Here, we extend this concept from inorganic 2D materials to 2D metal–organic frameworks (MOFs) that offer additional flexibility in realizing designer heterostructures. We successfully fabricate a monolayer 2D Cu-dicyanoanthracene MOF on a 2D van der Waals NbSe2 superconducting substrate. The structural and electronic properties of two different phases of the 2D MOF are characterized by low-temperature scanning tunneling microscopy (STM) and spectroscopy (STS), complemented by density-functional theory (DFT) calculations. These experiments allow us to follow the formation of the kagome band structure from Star of David-shaped building blocks. This work extends the synthesis and electronic tunability of 2D MOFs beyond the electronically less relevant metal and semiconducting surfaces to superconducting substrates, which are needed for the development of emerging quantum materials such as topological superconductors.

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Section: Introductionmentioning

confidence: 99%

Two-Dimensional Metal–Organic Framework on Superconducting NbSe₂

et al. 2021

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“…Starting from alcohols, such oxidation (or dehydrogenation reaction) is straightforward on copper surfaces − but also partially occurs on silver ,− and gold surfaces . A peculiar kind of alcohol, the hexahydroxytriphenylene (HHTP) molecule, has attracted much attention in this respect.…”

Section: Introductionmentioning

confidence: 99%

Role of the Structure and Reactivity of Cu and Ag Surfaces in the Formation of a 2D Metal–Hexahydroxytriphenylene Network

et al. 2021

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We have investigated the role played by the atomic structure and reactivity of the supporting Ag(111) and Cu(111) surfaces on the formation of 2D metal–organic networks (2D-MONs) involving metal adatom clusters spawned by these two surfaces. While the hexahydroxytriphenylene (HHTP) molecule forms complexes with Ag3 and Cu3 adatom clusters on, respectively, the Ag(111) and Cu(111) surfaces, an extended order is only observed in the 2D-MON on Ag(111). By combining scanning tunneling microscopy measurements, density functional theory calculations, and microscopy image simulations, we show that the formation of Ag–HHTP metal–organic complexes is structurally compatible with a periodic arrangement of HHTP on the Ag(111) surface. In contrast, on Cu(111), tightly bonded and localized Cu–HHTP motifs are stabilized by the interaction of Cu adclusters with HHTP. However, they cannot match the surface structure of Cu(111) to form an extended 2D-MON. We observed that the formation of large 2D-MON domains on a metallic surface is only possible when the periodicity of the adsorbed surface assembly is weakly perturbed by the addition of metal adclusters that reinforced the bonding.

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“…In our lattice, the Cu ions form a Kagomé network, but similar lattices were synthesized with Fe. [37,38] The adsorption of THQ molecules alone, [39] without metallic linker, leads to an ordered arrangement of organic molecules with no chemical reaction, i.e., no real chemical binding. The organic molecules stack together only via hydrogen bonds.…”

Section: Introductionmentioning

confidence: 99%

Self‐Organized Kagomé‐Lattice in a Conductive Metal‐Organic Monolayer

Shaiek

Denawi

Koudia

et al. 2022

Adv Materials Inter

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artificial monolayers each year, and a multitude of techniques like, e.g., molecular beam epitaxy, chemical deposition on surfaces, synthesis in wet environment and many others. Initially mainly studied for their fundamentally new and exotic properties, 2D materials have now attracted widespread interest due to their high potential for novel nanotechnological applications. [3][4][5][6][7][8][9] In this context, 2D materials composed of metal atoms and organic linkers have emerged as promising candidates to combine the advantages of both realms, also called 2D metal-organic frameworks (MOFs). For potential applications, we may cite, for example, their abilities in molecular recognition and functionalities for heterogeneous asymmetric catalysis, while their peculiar topological properties are interesting for new spintronic devices. [10][11][12][13][14][15][16][17][18] Most of the 2D metalorganic frameworks (MOFs) synthesized so far are almost perfect insulators but there is a major exception, namely the subclass of conductive MOFs or c-MOFs which are either metallic or at least semiconducting. The development of these c-MOFs is an important challenge for future decades due to their novel electronic, optical, mechanical, and catalytic properties. [19][20][21][22][23] Graphene is of fundamental interest since its linearly dispersing highly mobile electrons may be viewed as a 2D versionThe on-surface synthesis of metal-organic covalent coordination networks with a dense Kagomé lattice of metallic centers is reported. Tetrahydroxyquinone and metal atoms (M = Cu or Mn) are codeposited on Ag( 111) substrate to build well-ordered 2D lattices M 3 C 6 O 6 . The surface is studied by scanning tunneling microscopy, low-energy electron diffraction, and X-ray photoelectron spectroscopy (XPS). Density functional theory (DFT) reveals a Cu + charge state and no local magnetic moments for the Cu-organic network. For the Mn-organic network, the charge state Mn 2+ and a local spin S = 5/2 are found. Charge transfer stabilizes the Cu + and Mn 2+ charge states. DFT calculations show a Dirac point, i.e., a band crossing with linear electron dispersion at the K-point g g a b   (2 / 3) +(1/3) of the Brillouin zone. This Dirac point is at the Fermi level without charge transfer but drops by 100 meV if electron doping of Cu 3 C 6 O 6 on Ag(111) surface is acknowledged. The magnetic couplings of an isolated Mn 3 C 6 O 6 monolayer to be short range and antiferromagnetic leading to high frustration at the Kagomé lattice and a tendency toward a spin-liquid ground state are predicted. In the case of hole transfer from the substrate, ferromagnetic ordering is introduced, making Mn 3 C 6 O 6 an interesting candidate for the quantum anomalous Hall effect.

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Highly Degenerate Ground States in a Frustrated Antiferromagnetic Kagome Lattice in a Two-Dimensional Metal–Organic Framework

Cited by 30 publications

References 62 publications

Two-Dimensional Metal–Organic Framework on Superconducting NbSe₂

Two-Dimensional Metal–Organic Framework on Superconducting NbSe₂

Role of the Structure and Reactivity of Cu and Ag Surfaces in the Formation of a 2D Metal–Hexahydroxytriphenylene Network

Self‐Organized Kagomé‐Lattice in a Conductive Metal‐Organic Monolayer

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Highly Degenerate Ground States in a Frustrated Antiferromagnetic Kagome Lattice in a Two-Dimensional Metal–Organic Framework

Cited by 30 publications

References 62 publications

Two-Dimensional Metal–Organic Framework on Superconducting NbSe2

Two-Dimensional Metal–Organic Framework on Superconducting NbSe2

Role of the Structure and Reactivity of Cu and Ag Surfaces in the Formation of a 2D Metal–Hexahydroxytriphenylene Network

Self‐Organized Kagomé‐Lattice in a Conductive Metal‐Organic Monolayer

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Two-Dimensional Metal–Organic Framework on Superconducting NbSe₂

Two-Dimensional Metal–Organic Framework on Superconducting NbSe₂