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2D Magnetic Molecular Materials
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2D Magnetic Molecular Materials

A special issue of Molecules (ISSN 1420-3049). This special issue belongs to the section "Materials Chemistry".

Deadline for manuscript submissions: closed (31 March 2022) | Viewed by 7477

Special Issue Editors

Dr. Elena Bartolomé

E-Mail Website
Guest Editor
Department of Mechanical Engineering, School of Engineering, Escola Universitaria Salesiana de Sarrià (EUSS), Head of EUSS Research Group, Passeig Sant Joan Bosco, 74, 08017 Barcelona, Spain
Interests: molecular magnetism; multifunctional lanthanide-based single molecule magnets (SMMs); 4f/3d metal-organic frameworks (MOFs); 2D MOFs; magnetism of molecules on surfaces; phtalocyanines; magnetic wheels
Dr. Ana Arauzo

E-Mail Website
Guest Editor
Instituto de Nanociencia y Materiales de Aragón (INMA) and Departamento de Física de la Materia Condensada, CSIC- Universidad de Zaragoza, 50009 Zaragoza, Spain
Interests: molecular magnetism; molecular spintronics; luminescent SMMs; 2D magnetic molecular materials; hybrid applications; MOFs; magnetic materials; spin-glasses; thermophysical properties

Special Issue Information

Dear Colleagues,

2D molecular materials are receiving growing interest owing to their huge possibilities of application in electronics, spintronics, energy storage, catalysis, sensing, biomedicine, etc., and intriguing new physics appearing at the 2D limit, on interfaces and surfaces. The study of molecular magnetism in 2D materials based on transition metal (3d) and lanthanide (4f) ions is of particular interest. While most well-studied 2D materials are inorganic solids, like the very well-known graphene, recent advances in coordination chemistry have enabled the synthesis of 2D metal-organic frameworks (2D MOFs), which can be functionalized in a convenient way. Adequate exfoliation of these materials into nanosheets would allow the use these nano-objects in devices or heterostructures. Other attractive approaches towards achieving 2D molecular overlayers onto substrates include the grafting of molecules on functionalized surfaces, the use of surface-coordinated MOF thin films (SURMOFs), or the self-assembly of evaporated molecules. Different types of magnetic 2D MOFs are being investigated, such as materials with magnetic cooperativity, spin-crossover, magnetocaloric effect, and 2D MOFs with slow magnetic relaxation, where the nodes are either single-ion magnets (SIMs) or single-molecule magnets (SMMs), or which embed single-chain magnets (SCMs). SMM-2D MOFs represent ideal models to investigate magneto-structural properties, such as the occurrence of relaxation and quantum tunneling of the magnetization behavior under different coupling schemes between the magnetic sub-units, or the competition with magnetic ordering. The investigation of the magnetic properties of SIMs and SMMs onto surfaces, with potential application in molecular spintronics, high-density information storage and quantum computing, is also receiving considerable attention. Finally, a current challenge in the field is the development of multifunctional 2D molecular materials incorporating several properties such as, for instance, SMM behavior and luminescence.

This Special Issue will cover recent progress in all these topics, and other novel trends in the field of 2D magnetic molecular magnetism.

Dr. Elena Bartolomé
Dr. Ana Arauzo
Guest Editors

Manuscript Submission Information

Manuscripts should be submitted online at www.mdpi.com by registering and logging in to this website. Once you are registered, click here to go to the submission form. Manuscripts can be submitted until the deadline. All submissions that pass pre-check are peer-reviewed. Accepted papers will be published continuously in the journal (as soon as accepted) and will be listed together on the special issue website. Research articles, review articles as well as short communications are invited. For planned papers, a title and short abstract (about 100 words) can be sent to the Editorial Office for announcement on this website.

Submitted manuscripts should not have been published previously, nor be under consideration for publication elsewhere (except conference proceedings papers). All manuscripts are thoroughly refereed through a single-blind peer-review process. A guide for authors and other relevant information for submission of manuscripts is available on the Instructions for Authors page. Molecules is an international peer-reviewed open access semimonthly journal published by MDPI.

Please visit the Instructions for Authors page before submitting a manuscript. The Article Processing Charge (APC) for publication in this open access journal is 2700 CHF (Swiss Francs). Submitted papers should be well formatted and use good English. Authors may use MDPI's English editing service prior to publication or during author revisions.

Keywords

  • 2D metal-organic frameworks (2D MOFs) based on 3d/4f ions
  • Single-Molecule Magnet 2D metal-organic frameworks (SMM-2D MOFs)
  • Multifunctional 2D coordination polymers (e.g. luminescent SMMs)
  • Exfoliated magnetic nanosheets
  • 2D magnetic materials onto functionalized surfaces
  • Magnetism of surface-supported metal-organic frameworks (SURMOFs)
  • Magnetism of self-assembled molecular monolayers onto surfaces
  • 2D magnetic molecular heterostructures
  • Molecular spintronics
  • Molecular magnetic thin films

Published Papers (3 papers)

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Research

13 pages, 3019 KiB  
Article
Optimized Liquid-Phase Exfoliation of Magnetic van der Waals Heterostructures: Towards the Single Layer and Deterministic Fabrication of Devices
by Lucía Martín-Pérez and Enrique Burzurí
Molecules 2021, 26(23), 7371; https://0-doi-org.brum.beds.ac.uk/10.3390/molecules26237371 - 04 Dec 2021
Cited by 4 | Viewed by 2106
Abstract
Van der Waals magnetic materials are promising candidates for spintronics and testbeds for exotic magnetic phenomena in low dimensions. The two-dimensional (2D) limit in these materials is typically reached by mechanically breaking the van der Waals interactions between layers. Alternative approaches to producing [...] Read more.
Van der Waals magnetic materials are promising candidates for spintronics and testbeds for exotic magnetic phenomena in low dimensions. The two-dimensional (2D) limit in these materials is typically reached by mechanically breaking the van der Waals interactions between layers. Alternative approaches to producing large amounts of flakes rely on wet methods such as liquid-phase exfoliation (LPE). Here, we report an optimized route for obtaining monolayers of magnetic cylindrite by LPE. We show that the selection of exfoliation times is the determining factor in producing a statistically significant amount of monolayers while keeping relatively big flake areas (~1 µm2). We show that the cylindrite lattice is preserved in the flakes after LPE. To study the electron transport properties, we have fabricated field-effect transistors based on LPE cylindrite. Flakes are deterministically positioned between nanoscale electrodes by dielectrophoresis. We show that dielectrophoresis can selectively move the larger flakes into the devices. Cylindrite nanoscale flakes present a p-doped semiconducting behaviour, in agreement with the mechanically exfoliated counterparts. Alternating current (AC) admittance spectroscopy sheds light on the role played by potential barriers between different flakes in terms of electron transport properties. The present large-scale exfoliation and device fabrication strategy can be extrapolated to other families of magnetic materials. Full article
(This article belongs to the Special Issue 2D Magnetic Molecular Materials)
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26 pages, 2765 KiB  
Article
Slow Magnetic Relaxation in {[CoCxAPy)] 2.15 H2O}n MOF Built from Ladder-Structured 2D Layers with Dimeric SMM Rungs
by Ana Arauzo, Elena Bartolomé, Javier Luzón, Pablo J. Alonso, Angelica Vlad, Maria Cazacu, Mirela F. Zaltariov, Sergiu Shova, Juan Bartolomé and Constantin Turta
Molecules 2021, 26(18), 5626; https://0-doi-org.brum.beds.ac.uk/10.3390/molecules26185626 - 16 Sep 2021
Cited by 3 | Viewed by 2028
Abstract
We present the magnetic properties of the metal-organic framework {[CoCxAPy]·2.15 H2O}n (Cx = bis(carboxypropyl)tetramethyldisiloxane; APy = 4,4`-azopyridine) (1) that builds up from the stacking of 2D coordination polymers. The 2D-coordination polymer in the bc plane is formed by [...] Read more.
We present the magnetic properties of the metal-organic framework {[CoCxAPy]·2.15 H2O}n (Cx = bis(carboxypropyl)tetramethyldisiloxane; APy = 4,4`-azopyridine) (1) that builds up from the stacking of 2D coordination polymers. The 2D-coordination polymer in the bc plane is formed by the adjacent bonding of [CoCxAPy] 1D two-leg ladders with Co dimer rungs, running parallel to the c-axis. The crystal packing of 2D layers shows the presence of infinite channels running along the c crystallographic axis, which accommodate the disordered solvate molecules. The Co(II) is six-coordinated in a distorted octahedral geometry, where the equatorial plane is occupied by four carboxylate oxygen atoms. Two nitrogen atoms from APy ligands are coordinated in apical positions. The single-ion magnetic anisotropy has been determined by low temperature EPR and magnetization measurements on an isostructural compound {[Zn0.8Co0.2CxAPy]·1.5 CH3OH}n (2). The results show that the Co(II) ion has orthorhombic anisotropy with the hard-axis direction in the C2V main axis, lying the easy axis in the distorted octahedron equatorial plane, as predicted by the ab initio calculations of the g-tensor. Magnetic and heat capacity properties at very low temperatures are rationalized within a S* = 1/2 magnetic dimer model with anisotropic antiferromagnetic interaction. The magnetic dimer exhibits slow relaxation of the magnetization (SMM) below 6 K in applied field, with a tlf ≈ 2 s direct process at low frequencies, and an Orbach process at higher frequencies with U/kB = 6.7 ± 0.5 K. This compound represents a singular SMM MOF built-up of Co-dimers with an anisotropic exchange interaction. Full article
(This article belongs to the Special Issue 2D Magnetic Molecular Materials)
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14 pages, 40686 KiB  
Article
Luminescent and Magnetic Tb-MOF Flakes Deposited on Silicon
by Elena Bartolomé, Ana Arauzo, Sergio Herce, Anna Palau, Narcis Mestres, Sara Fuertes, Pablo Sevilla, Nicholas S. Settineri, Laura Navarro-Spreafico, Jonay González and E. Carolina Sañudo
Molecules 2021, 26(18), 5503; https://0-doi-org.brum.beds.ac.uk/10.3390/molecules26185503 - 10 Sep 2021
Cited by 6 | Viewed by 2463
Abstract
The synthesis of a terbium-based 2D metal–organic framework (MOF), of formula [Tb(MeCOO)(PhCOO)2] (1), a crystalline material formed by neutral nanosheets held together by Van der Waals interactions, is presented. The material can be easily exfoliated by sonication and deposited [...] Read more.
The synthesis of a terbium-based 2D metal–organic framework (MOF), of formula [Tb(MeCOO)(PhCOO)2] (1), a crystalline material formed by neutral nanosheets held together by Van der Waals interactions, is presented. The material can be easily exfoliated by sonication and deposited onto different substrates. Uniform distributions of Tb-2D MOF flakes onto silicon were obtained by spin-coating. We report the luminescent and magnetic properties of the deposited flakes compared with those of the bulk. Complex 1 is luminescent in the visible and has a sizeable quantum yield of QY = 61% upon excitation at 280 nm. Photoluminescence measurements performed using a micro-Raman set up allowed us to characterize the luminescent spectra of individual flakes on silicon. Magnetization measurements of flakes-on-silicon with the applied magnetic field in-plane and out-of-plane display anisotropy. Ac susceptibility measurements show that 1 in bulk exhibits field-induced slow relaxation of the magnetization through two relaxation paths and the slowest one, with a relaxation time of τlf ≈ 0.5 s, is assigned to a direct process mechanism. The reported exfoliation of lanthanide 2D-MOFs onto substrates is an attractive approach for the development of multifunctional materials and devices for different applications. Full article
(This article belongs to the Special Issue 2D Magnetic Molecular Materials)
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