Tuning Molecule-Mediated Spin Coupling in Bottom-Up-Fabricated Vanadium-Tetracyanoethylene Nanostructures

Wegner, Daniel; Yamachika, Ryan; Zhang, Xiaowei; Wang, Yayu; Baruah, Tunna; Pederson, Mark R.; Bartlett, Bart M.; Long, Jeffrey R.; Crommie, Michael F.

doi:10.1103/physrevlett.103.087205

Cited by 60 publications

(56 citation statements)

References 28 publications

(32 reference statements)

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“…Our observations thus indicate that the screened spin is not localized on the metal ion, contrary to conclusions generally drawn from molecular junction experiments [1][2][3] and studies of metal-organic complexes at surfaces 16,18,19,23,24 , but induced by charge transfer into molecular ligand states 13,[25][26][27][28] , independently of the spin of the pristine molecules.…”

Section: I/dvcontrasting

confidence: 56%

Spin coupling and relaxation inside molecule–metal contacts

et al. 2011

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Advances in molecular electronics depend on the ability to control the charge and spin of single molecules at the interface with a metal. Here we show that bonding of metal-organic complexes to a metallic substrate induces the formation of coupled metal-ligand spin states, increasing the spin degeneracy of the molecules and opening multiple spin relaxation channels. scanning tunnelling spectroscopy reveals the sign and magnitude of intramolecular exchange coupling as well as the orbital character of the spin-polarized molecular states. We observe coexisting Kondo, spin, and vibrational inelastic channels in a single molecule, which lead to pronounced intramolecular variations of the conductance and spin dynamics. The spin degeneracy of the molecules can be controlled by artificially fabricating molecular clusters of different size and shape. By comparing data for vibronic and spin-exchange excitations, we provide a positive test of the universal scaling properties of inelastic Kondo processes having different physical origin.

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Section: I/dvcontrasting

confidence: 56%

Spin coupling and relaxation inside molecule–metal contacts

et al. 2011

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“…33,34 However, to our knowledge, no extended purely 2D network has been reported using TCNE, and only the bottom-up fabrication by atomic manipulation of small V-TCNE clusters on Ag(100) has been reported. 35 Our results suggest that during the growth of TCNE coordination material by Chemical Vapor Deposition methods for organic magnetic applications, possible substitution of the magnetic metal centers by non-magnetic substrate adatoms might lead to weaker magnetic responses.…”

Section: Discussionmentioning

confidence: 99%

Temperature-controlled metal/ligand stoichiometric ratio in Ag-TCNE coordination networks

Rodrı́guez-Fernández

Lauwaet

Herranz

et al. 2015

The Journal of Chemical Physics

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The deposition of tetracyanoethylene (TCNE) on Ag(111), both at Room Temperature (RT, 300 K) and low temperatures (150 K), leads to the formation of coordination networks involving silver adatoms, as revealed by Variable-Temperature Scanning Tunneling Microscopy. Our results indicate that TCNE molecules etch away material from the step edges and possibly also from the terraces, which facilitates the formation of the observed coordination networks. Moreover, such process is temperature dependent, which allows for different stoichiometric ratios between Ag and TCNE just by adjusting the deposition temperature. X-ray Photoelectron Spectroscopy and Density Functional Theory calculations reveal that charge-transfer from the surface to the molecule and the concomitant geometrical distortions at both sides of the organic/inorganic interface might facilitate the extraction of silver atoms from the step-edges and, thus, its incorporation into the observed TCNE coordination networks. C 2015 AIP Publishing LLC. [http://dx

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“…8À10 Prominent results include multicomponent two-dimensional metalÀ organic networks 11,12 or dense-packed arrays of metalÀorganic complexes, 2,13 where unpaired d-or f-electrons contribute to the magnetic moment for transition metal and lanthanide centers, respectively. This selfassembly approach guarantees an exquisite control on the positions and the local coordination sphere of the magnetic centers, comparable to the precise atom positioning achieved by serial manipulation procedures based on low-temperature scanning tunneling microscopy (STM), 14,15 which however are not applicable for large-scale patterning of substrates, a frequent criterion for applications.…”

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confidence: 99%

Restoring the Co Magnetic Moments at Interfacial Co-Porphyrin Arrays by Site-Selective Uptake of Iron

et al. 2015

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T he fabrication of addressable, surfacebased arrays comprising single atomic spins and magnetic moments is a key to comprehensively understand magnetic phenomena on the nanoscale, 1À3 and to realize potential sensing, information storage, spintronic or quantum computing devices. 4À7 Recently, the bottom-up assembly of metalÀorganic magnetic layers and architectures on surfaces has attracted considerable interest, given the versatility of molecular building blocks combined with metal centers featuring magnetic moments. 8À10 Prominent results include multicomponent two-dimensional metalÀ organic networks 11,12 or dense-packed arrays of metalÀorganic complexes, 2,13 where unpaired d-or f-electrons contribute to the magnetic moment for transition metal and lanthanide centers, respectively. This selfassembly approach guarantees an exquisite control on the positions and the local coordination sphere of the magnetic centers, comparable to the precise atom positioning achieved by serial manipulation procedures based on low-temperature scanning tunneling microscopy (STM), 14,15 which however are not applicable for large-scale patterning of substrates, a frequent criterion for applications.Commonly, the interaction of molecules and metal centers with the supporting surface affects their electronic and magnetic properties, and tetrapyrrole species have been frequently employed for exemplary investigations in this context. 16 While this complemented by density functional theory (DFT) calculations, evidence a ferromagnetic coupling between the Fe and the Co center concomitant with a complex charge redistribution involving the porphyrin ligand. Thus, we demonstrate an unusual metalloporphyrin coordination geometry that opens pathways to spatially order and engineer magnetic moments in surface-based nanostructures.KEYWORDS: magnetochemistry . magnetic moment . metalloporphyrin . template . scanning tunneling microscopy (STM) . X-ray magnetic circular dichroism (XMCD) . density functional theory (DFT) ARTICLE

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Tuning Molecule-Mediated Spin Coupling in Bottom-Up-Fabricated Vanadium-Tetracyanoethylene Nanostructures

Cited by 60 publications

References 28 publications

Spin coupling and relaxation inside molecule–metal contacts

Spin coupling and relaxation inside molecule–metal contacts

Temperature-controlled metal/ligand stoichiometric ratio in Ag-TCNE coordination networks

Restoring the Co Magnetic Moments at Interfacial Co-Porphyrin Arrays by Site-Selective Uptake of Iron

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