Monolayer and Multilayer Films of [Mn12O12(O2CMe)16]

Steckel, Jonathan S.; Persky, Nicole S.; Martinez, Chelsea R.; Barnes, Calvin L.; Fry, Elizabeth A.; Kulkarni, J.A.; Burgess, James D.; Pacheco, Rachel B.; Stoll, Sarah L.

doi:10.1021/nl0343553

Cited by 53 publications

(32 citation statements)

References 23 publications

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“…Demonstrating that taking advantage of the large lability of the acetate ligand, Mn 12 -acetate can be attached potentially to any surface covered with carboxylate groups [50]. Similar results were obtained by Bucher and co-workers using a Mn 12 -pivalate derivative [51,52].…”

Section: Deposition and Organization Of Smms On Surfacessupporting

confidence: 76%

Magnetic molecular nanostructures: Design of magnetic molecular materials as monolayers, multilayers and thin films

Coronado

Martí‐Gastaldo

Tatay

2007

Applied Surface Science

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Section: Deposition and Organization Of Smms On Surfacessupporting

confidence: 76%

Magnetic molecular nanostructures: Design of magnetic molecular materials as monolayers, multilayers and thin films

Coronado

Martí‐Gastaldo

Tatay

2007

Applied Surface Science

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“…[2][3][4][5] Charged macromolecules, also known as polyelectrolytes, adsorb easily onto surfaces due to electrostatic, van der Waals, and/or hydrogen-bonding interactions. This makes them ideal candidates as a molecular glue to build complex functional systems in a layer-by-layer fashion, such as magnetic [6] and catalytic [7] films, memoryswitching devices, [8] nacre mimics, [9] optical coatings, [10] superhydrophobic [11] and biocompatible active [12,13] surfaces, photoactive systems, [14] carbon nanotube assemblies, [15] and so on.[4]Attempts to laterally control the size of such assemblies have been previously reported, but have so far been limited to the micrometer-scale and above. [16] Of challenging interest would be to succeed in controlling multilayer build-up in the nanometer range, when the size of the macromolecules is similar to the size of the objects to be built.…”

mentioning

confidence: 99%

Nanoconfined Polyelectrolyte Multilayers

et al. 2006

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The self-assembly of nanometer-sized objects into larger ensembles is an efficient way to fabricate complex functional nanosystems.[1] A typical example of such assembling strategies is the layer-by-layer adsorption of charged macromolecules of alternate sign to give rise to multilayered films of a complex vertical architecture. These can incorporate proteins, inorganic clusters and platelets, C 60 , dyes, conducting polymers, DNA, and even viruses. [2][3][4][5] Charged macromolecules, also known as polyelectrolytes, adsorb easily onto surfaces due to electrostatic, van der Waals, and/or hydrogen-bonding interactions. This makes them ideal candidates as a molecular glue to build complex functional systems in a layer-by-layer fashion, such as magnetic [6] and catalytic [7] films, memoryswitching devices, [8] nacre mimics, [9] optical coatings, [10] superhydrophobic [11] and biocompatible active [12,13] surfaces, photoactive systems, [14] carbon nanotube assemblies, [15] and so on.[4]Attempts to laterally control the size of such assemblies have been previously reported, but have so far been limited to the micrometer-scale and above. [16] Of challenging interest would be to succeed in controlling multilayer build-up in the nanometer range, when the size of the macromolecules is similar to the size of the objects to be built. This would allow the creation of three-dimensional nano-objects that have a vertical composition controlled by the succession of adsorption events, and of a lateral size identical to those of typical macromolecules. In contrast to current nanofabrication technologies, [17] these systems would permit the incorporation of the vast library of currently existing soft-matter objects. From a more basic point of view, decreasing the lateral size of multilayers in the nanometer range is expected to perturb the conformations of the macromolecules, which offers a supplementary tool to tune the properties of the system. Usually, global control over the conformation of charged chains can be performed by adjusting the ionic strength of the solutions, to screen electrostatic interactions between charged units.[18]However, local control of chain conformation has never been attained despite its basic and practical interests for, e.g., biomineralization, [19] biocompatibility and fouling issues, and for biosensing applications. [20,21] Here, lateral (horizontal) control over the growth of such self-assembled multilayers, down to dimensions smaller than the typical size of the macromolecular chains, is demonstrated. In addition, the conformations of the adsorbed macromolecules are shown to be strongly perturbed with respect to the usual, macroscopic case, due to self-confinement in restricted spaces. Apart from opening large perspectives for the fabrication of complex three-dimensional soft and hybrid nanostructures, the results indicate that conformations of macromolecules may be locally tuned by the proper design of the surfaces on which they adsorb. Here, the focus is on model chains that consist of two stron...

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“…The sample SMM 19,20 has the chemical formula [Fe 4 (L) 2 (dpm) 6 ], where Hdpm and H 3 L are dipivaloylmethane and the triol ligand, 11-(acetylthio)-2,2-bis(hydroxymethyl)undecanol, respectively. This Fe 4 molecule contains a magnetic tetrairon(III) core with long aliphatic chains terminated with thioacetyl groups ( Fig.…”

Section: Methodsmentioning

confidence: 99%

Effect of Aqueous Environment on Monolayer of Tetrairon(III) Single Molecule Magnet

Kanata

Nishino

Aoki

2012

J. Electrochem. Soc.

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A self-assembled monolayer (SAM) of a single molecule magnet (SMM) bearing a tetrairon(III) core and sulfur-containing terminal groups was exposed to aqueous solution. The effect of the chemical environment on the monolayer was investigated using cyclic voltammetry, X-ray photoelectron spectroscopy, and atomic force microscopy. The physisorbed SMM molecules desorbed and the sulfur atoms in the remaining SMM were oxidized during immersion in H 2 O, while the Fe(III) ions remained intact. We found that the SMM molecules concomitantly formed aggregates on the surface. These transformations caused significant changes to the redox properties of the SMM. The present research highlights the fragile nature of the SMM SAM against particular chemical environments and provides important insights into the exploitation of surface-tethered SMMs for a variety of applications.Single molecule magnets (SMMs) are a unique class of functional molecules. They possess versatile magnetic properties and show rich quantum behavior such as magnetic hysteresis of a molecular origin 1 and quantum tunneling of magnetization. 2 Since the first discovery of molecular magnetism in [Mn 12 (OAc) 16 (H 2 O) 4 O 12 ] (Mn 12 acetate), 3 SMMs have attracted considerable interest because of their potential for information storage device applications. In addition, SMMs offer a peculiar opportunity to explore magnetism at the nanoscale. Because it is desirable to immobilize SMM molecules on a solid surface to utilize and probe their magnetism, many studies have been devoted to create two-dimensional assemblies of SMMs. Several different approaches have been reported to deposit Mn 12 acetate, which is the archetypal SMM, on substrates including stamp-assisted deposition on a Si substrate, 4 immobilization by ligand-exchange on the surfaces of self-assembled monolayers (SAMs), 5-9 and grafting via electrostatic interactions. 10 Moreover, direct deposition onto metal surfaces can be achieved using organosulfur derivatives of Mn 12 acetate. 11-14 It is important to retain the useful magnetic properties for these surfacetethered SMMs. However, it is known that the Mn 12 acetate loses the useful magnetic property on a solid surface due to the structural instability of its inorganic core in the highly strained surface environment. [15][16][17][18] To avoid this, a different class of SMMs featuring tetrairon(III) cores (Fe 4 ) has been developed. It has recently proven that Fe 4 SMMs are sufficiently chemically robust to maintain magnetic hysteresis after direct deposition. 19,20 Besides developing methodology for surface immobilization, the practical application of SMMs requires an understanding of the chemical stability of their surface assembly against various chemical environments. Although the characterization of such stability is very important given the intrinsically fragile nature of SMMs, the available knowledge on this subject is quite limited. Currently the peculiar properties of SMMs emerge only at low temperatures, and this fact hampers their utili...

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Monolayer and Multilayer Films of [Mn₁₂O₁₂(O₂CMe)₁₆]

Cited by 53 publications

References 23 publications

Magnetic molecular nanostructures: Design of magnetic molecular materials as monolayers, multilayers and thin films

Magnetic molecular nanostructures: Design of magnetic molecular materials as monolayers, multilayers and thin films

Nanoconfined Polyelectrolyte Multilayers

Effect of Aqueous Environment on Monolayer of Tetrairon(III) Single Molecule Magnet

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