Electrostatic Spin Crossover in a Molecular Junction of a Single-Molecule MagnetFe2

AbstractThis issue of MRS Bulletin on molecular transport junctions highlights the current experimental and theoretical understanding of molecular charge transport and its extension to the rapidly growing areas of molecular and carbon nanotube electronics. This introduction will outline the progress that has been made in understanding the mechanisms of molecular junction transport and the challenges and future directions in exploring charge transport on the molecular scale. In spite of the substantial challenges, molecular charge transport is of great interest for its intrinsic importance to potential single-molecule electronic, thin-film electronic, and optoelectronic applications.

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A mononuclear five-coordinate Co(ii) single molecule magnet with a spin crossover between the S = 1/2 and 3/2 states

Dalton Transactions ◽

10.1039/c8dt03783c ◽

2018 ◽

Vol 47 (46) ◽

pp. 16596-16602 ◽

Cited By ~ 16

Author(s):

Lei Chen ◽

Jingbo Song ◽

Wen Zhao ◽

Gangji Yi ◽

Zhikuan Zhou ◽

...

Keyword(s):

Hysteresis Loop ◽

Single Molecule ◽

Magnetic Relaxation ◽

Spin Crossover ◽

Spin Transition ◽

Single Molecule Magnet ◽

Pyramidal Geometry ◽

Mononuclear Cobalt ◽

Slow Magnetic Relaxation ◽

Square Pyramidal Geometry

A mononuclear cobalt(ii) complex with square pyramidal geometry displays a spin transition with a small hysteresis loop and slow magnetic relaxation.

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Electrical control over the Fe(II) spin crossover in a single molecule: Theory and experiment

Physical Review B ◽

10.1103/physrevb.83.245415 ◽

2011 ◽

Vol 83 (24) ◽

Cited By ~ 144

Author(s):

V. Meded ◽

A. Bagrets ◽

K. Fink ◽

R. Chandrasekar ◽

M. Ruben ◽

...

Keyword(s):

Single Molecule ◽

Spin Crossover ◽

Electrical Control ◽

Theory And Experiment

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Molecular direction dependence of single-molecule conductance of a helical peptide in molecular junction

Physical Chemistry Chemical Physics ◽

10.1039/c2cp43499g ◽

2013 ◽

Vol 15 (3) ◽

pp. 757-760 ◽

Cited By ~ 29

Author(s):

Hirotaka Uji ◽

Tomoyuki Morita ◽

Shunsaku Kimura

Keyword(s):

Single Molecule ◽

Molecular Junction ◽

Helical Peptide ◽

Direction Dependence

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First-Principles Investigations of Magnetic Anisotropy and Spin-Crossover Behavior of Fe(III)-TBP Complexes

10.26434/chemrxiv.13110212.v1 ◽

2020 ◽

Author(s):

Rishu Khurana ◽

Sameer Gupta ◽

Md. Ehesan Ali

Keyword(s):

Single Molecule ◽

First Principles ◽

Density Functional ◽

Spin Crossover ◽

Zero Field ◽

Spin States ◽

Zero Field Splitting ◽

Field Splitting ◽

B3lyp Functional ◽

D Values

<div>With the ongoing efforts to obtain mononuclear 3d-transition metal complexes that manifest slow relaxation of magnetization and hence, can behave as single molecule magnets (SMMs), we have modelled 14 novel Fe(III) complexes out of which nine behave as potential SMMs. These complexes possess large zero-field splitting (ZFS)</div><div>parameter D in the range of -40 to -60 cm<sup>-1</sup>. The first-principles investigation of the ground-spin state applying density functional theory (DFT) and wave-function based</div><div>multi-configurations methods e.g. SA-CASSCF/NEVPT2 are found to be quite consistent except for few delicate cases with near degenerate spin-states. In such cases, the</div><div>hybrid B3LYP functional is found to be biased towards high-spin (HS) state. Altering the percentage of exact exchange admixed in B3LYP functional leads to intermediate spin</div><div>(IS) ground state consistent with the multireference calculations. The origin of large zero field splitting (ZFS) in the Fe(III)-based trigonal bipyramidal (TBP) complexes</div><div>is investigated and the D-values are further tuned by varying the axial ligands with group XV elements (N, P and As) and equatorial halide ligands from F, Cl, Br and I. Furthermore, a number of complexes are identified with very small Gibbs free energy values indicating the possible spin-crossover phenomenon between the bi-stable spin-states.</div>

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Addressing single spin crossover molecules in a two-dimensional monolayer

10.21203/rs.3.rs-251042/v1 ◽

2021 ◽

Author(s):

Yongfeng Tong ◽

Massine Kelaï ◽

Kaushik Bairagi ◽

Vincent Repain ◽

Jérôme Lagoute ◽

...

Keyword(s):

Spin State ◽

Single Molecule ◽

Spin Crossover ◽

Cooperative Behaviour ◽

Spintronic Devices ◽

Single Spin ◽

Elastic Interactions ◽

Molecular Spin ◽

External Stimuli ◽

At Will

Abstract Bistable spin-crossover molecules are particularly interesting to the development of innovative electronic and spintronic devices as they present two spin states that can be controlled by external stimuli. In this purpose, being able to switch at will the spin state of a single molecule in a dense molecular array is a key milestone. However, the elastic interactions between the molecules favour more cooperative behaviour where patches of neighbouring molecules switches simultaneously. We demonstrate here that the interaction of iron II spin-crossover molecules with a metallic substrate can strongly reduce their cooperative behaviour until addressing independently single molecular spin state. Mechanoelastic model is able to reproduce well such findings.

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Electroswitching of the single-molecule magnet behaviour in an octahedral spin crossover cobalt(ii) complex with a redox-active pyridinediimine ligand

Chemical Communications ◽

10.1039/d0cc03357j ◽

2020 ◽

Vol 56 (81) ◽

pp. 12242-12245

Author(s):

Renato Rabelo ◽

Luminita Toma ◽

Nicolás Moliner ◽

Miguel Julve ◽

Francesc Lloret ◽

...

Keyword(s):

Single Molecule ◽

Spin Crossover ◽

Single Molecule Magnet ◽

Redox Active

A unique example of electroswitchable spin crossover molecular nanomagnet which proceeds through one-electron oxidation of the slow-relaxing paramagnetic low-spin CoII ion (SCo = 1/2, ON) to the diamagnetic low-spin CoIII ion (SCo = 0, OFF).

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Robust spin crossover and memristance across a single molecule

Nature Communications ◽

10.1038/ncomms1940 ◽

2012 ◽

Vol 3 (1) ◽

Cited By ~ 321

Author(s):

Toshio Miyamachi ◽

Manuel Gruber ◽

Vincent Davesne ◽

Martin Bowen ◽

Samy Boukari ◽

...

Keyword(s):

Single Molecule ◽

Spin Crossover

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Optical probes of molecules as nano-mechanical switches

Nature Communications ◽

10.1038/s41467-020-19703-y ◽

2020 ◽

Vol 11 (1) ◽

Author(s):

Dean Kos ◽

Giuliana Di Martino ◽

Alexandra Boehmke ◽

Bart de Nijs ◽

Dénes Berta ◽

...

Keyword(s):

Molecular Electronics ◽

Single Molecule ◽

Electrical Transport ◽

Density Functional ◽

Information Technologies ◽

Electronic Device ◽

Density Functional Theory Calculations ◽

Molecular Junction ◽

Single Molecule Level ◽

Ultralow Energy

AbstractMolecular electronics promises a new generation of ultralow-energy information technologies, based around functional molecular junctions. Here, we report optical probing that exploits a gold nanoparticle in a plasmonic nanocavity geometry used as one terminal of a well-defined molecular junction, deposited as a self-assembled molecular monolayer on flat gold. A conductive transparent cantilever electrically contacts individual nanoparticles while maintaining optical access to the molecular junction. Optical readout of molecular structure in the junction reveals ultralow-energy switching of ∼50 zJ, from a nano-electromechanical torsion spring at the single molecule level. Real-time Raman measurements show these electronic device characteristics are directly affected by this molecular torsion, which can be explained using a simple circuit model based on junction capacitances, confirmed by density functional theory calculations. This nanomechanical degree of freedom is normally invisible and ignored in electrical transport measurements but is vital to the design and exploitation of molecules as quantum-coherent electronic nanodevices.

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