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Single-Molecule Magnets on Surfaces

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Molecular Nanomagnets and Related Phenomena

Part of the book series: Structure and Bonding ((STRUCTURE,volume 164))

Abstract

Encoding and manipulating information through the spin degrees of freedom of individual magnetic molecules or atoms is one of the central challenges in the continuing trend towards molecular/atomic scale electronics. With their large magnetic moment and long spin relaxation time, single-molecule magnets (SMMs) are of special importance in this emerging field. Their electrical addressing at the molecular level appears now well within reach using STM methods, which require to organize SMMs on a conducting surface. In this chapter, we present a critical overview of the latest achievements in the deposition of SMMs as monolayers or submonolayers on native or prefunctionalized surfaces. Special emphasis is placed on the selection and design of molecular structures that withstand solution or vapour-phase processing and that maintain their magnetic functionality on a surface. Chemical strategies to control the strength of molecule–substrate interaction and the molecular orientation on the surface are also illustrated. Rewardingly, these efforts have shown that the distinctive properties of SMMs, i.e. slow spin relaxation and quantum tunnelling of the magnetic moment, persist in metal-wired molecules.

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Notes

  1. 1.

    In 2009, Journal of Materials Chemistry has published a themed issue on molecular spintronics and quantum computing. See ref. [12].

  2. 2.

    Here we adopt Rinehart definition of T B as the temperature affording a relaxation time of 100 s in zero applied field. The need for a reference relaxation time arises from the fact that different techniques have different measurement times and, consequently, detect blocking of the magnetic moment at different temperatures.

  3. 3.

    Projection coefficients define the relationship between local anisotropic contributions (among which single-ion terms) and the overall anisotropy (D) associated with each total spin state. They can be computed using recursive relations. For details see [23].

  4. 4.

    In an XMCD experiment, absorption cross sections for photon helicity parallel (σ+) and antiparallel (σ−) to the applied field are separately measured and the XMCD signal is defined as the difference (σ− − σ+). It is usually expressed as percentage of the maximum in the isotropic spectrum, that can be estimated as (σ+ + σ−)/2 in the case of transition metals. Since the isotropic spectrum intensity is proportional to the number of absorbing atoms, the XMCD signal so defined (XMCD%) provides the dichroic response per atom.

  5. 5.

    Similar complexes can also be prepared in a single step, as described for related systems containing acetylacetonato ligands [131].

  6. 6.

    In the absence of superexchange interactions and saturation effects, both the overall magnetization (as probed by traditional magnetometry) and the local magnetic polarizations at metal sites (as probed by XMCD) follow the Curie law. When superexchange interactions are switched on, the local magnetic polarizations are not necessarily proportional to each other and to molecular magnetization [147, 153]. In Fe3Cr systems, the magnetic polarization at Fe sites is always parallel to the applied field, while that at the Cr site must switch from field antiparallel to field parallel with increasing T. The corresponding XMCD signals are thus expected to exhibit completely different T dependences. Notice that in the temperature range of interest magnetic anisotropy has no effect on magnetic behaviour and can be neglected.

  7. 7.

    While XMCD utilizes circularly polarized X-rays to study magnetism, XNLD uses linearly polarized radiation to probe structural order. In an XNLD experiment, the beam is tilted from the surface normal and the XNLD signal is defined as the difference in response to vertically (σV) and horizontally (σH) polarized radiation, (σV−σH). Normalization of the XNLD signal is carried out as described for XMCD (see footnote 3).

Abbreviations

4-mobca:

4′-Mercapto-octafluorobiphenyl-4-carboxylic acid

4-mtba:

4-Mercapto-tetrafluorobenzoic acid

AC:

Alternating current

DFT:

Density functional theory

DPN:

Dip-pen nanolithography

EPR:

Electron paramagnetic resonance

ESI-MS:

Electrospray ionization mass spectrometry

Et-saoH2 :

2-Hydroxyphenylpropanone oxime

H2hmb:

N′-(2-hydroxy-3-methoxybenzylidene)benzhydrazide

H2Pc:

Phthalocyanine

H2sao:

2-Hydroxybenzaldehyde oxime

Hbiph:

Biphenyl-4-carboxylic acid

Hdmbz:

3,5-Dimethylbenzoic acid

Hdpm:

Dipivaloylmethane

Hhfac:

Hexafluoroacetylacetone

HOPG:

Highly oriented pyrolitic graphite

Hpfb:

4-Fluorobenzoic acid

Hpta:

Pivaloyl trifluoromethyl acetone

Hth:

3-Thiophene-carboxylic acid

Htpc:

p-Terphenyl-4-carboxylic acid

LnDD:

Lanthanide double-decker

ML:

Monolayer

NP:

Nanoparticle

PyNO:

Pyridine N-oxide

QT:

Quantum tunnelling

SAM:

Self-assembled monolayer

SH:

Spin hamiltonian

SMM:

Single-molecule magnet

SQUID:

Superconducting quantum interference device

STM:

Scanning tunnelling microscope/scanning tunnelling microscopy

STS:

Scanning tunnelling spectroscopy

T B :

Blocking temperature

TEY:

Total electron yield

ToF-SIMS:

Time of flight secondary ion mass spectrometry

UHV:

Ultra-high vacuum

VSM:

Vibrating sample magnetometer

XAS:

X-ray absorption spectroscopy

XMCD:

X-ray magnetic circular dichroism

XNLD:

X-ray natural linear dichroism

XPS:

X-ray photoelectron spectroscopy

ZFS:

Zero-field splitting

μSR:

Muon spin relaxation

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Acknowledgments

We are indebted to many colleagues that have substantially contributed to our scientific activity over the years. We especially wish to thank Dante Gatteschi, Roberta Sessoli and Andrea Caneschi (Università degli Studi di Firenze and INSTM Research Unit of Firenze, Sesto Fiorentino, Italy) as invaluable teachers and endless sources of ideas and illuminating suggestions. Many groundbreaking experiments were only possible thanks to Wolfgang Wernsdorfer (Institut Néel-CNRS, Grenoble, France), Anne-Laure Barra (LNCMI-CNRS, Grenoble, France), Philippe Sainctavit (IMPMC, Université Pierre et Marie Curie, Paris, France) and Zaher Salman (PSI, Villigen, Switzerland). This work was financially supported by European Union through an ERANET project “NanoSci-ERA: Nanoscience in European Research Area” (SMMTRANS), by European Research Council through the Advanced Grant MolNanoMas (267746) and by Italian MIUR through PRIN (2008FZK5AC) and FIRB (RBAP117RWN, RBFR10OAI0) projects.

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  1. Dipartimento di Scienze Chimiche e Geologiche, Università degli Studi di Modena e Reggio Emilia & INSTM Research Unit of Modena and Reggio Emilia, Via G. Campi 183, 41125, Modena, Italy

    Andrea Cornia

  2. Dipartimento di Chimica “Ugo Schiff”, Università degli Studi di Firenze & INSTM Research Unit of Firenze, Via della Lastruccia 3-13, 50019, Sesto Fiorentino, (FI), Italy

    Matteo Mannini

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Correspondence to Andrea Cornia .

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  1. Coll. of Chemistry and Molecular Eng., Peking University, Beijing, China

    Song Gao

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Cornia, A., Mannini, M. (2014). Single-Molecule Magnets on Surfaces. In: Gao, S. (eds) Molecular Nanomagnets and Related Phenomena. Structure and Bonding, vol 164. Springer, Berlin, Heidelberg. https://doi.org/10.1007/430_2014_150

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