scholarly journals Ab Initio Prediction of High-Temperature Magnetic Relaxation Rates in Single-Molecule Magnets

2021 ◽  
Vol 143 (15) ◽  
pp. 5943-5950
Author(s):  
Daniel Reta ◽  
Jon G. C. Kragskow ◽  
Nicholas F. Chilton
Keyword(s):  
High Temperature ◽  
Ab Initio ◽  
Single Molecule ◽  
Magnetic Relaxation ◽  
Relaxation Rates ◽  
Single Molecule Magnets ◽  
Ab Initio Prediction

scholarly journals Ab Initio Prediction of High-Temperature Magnetic Relaxation Rates in Single-Molecule Magnets

2021 ◽  
Author(s):  
Daniel Reta ◽  
Jon G. C. Kragskow ◽  
Nicholas Chilton
Keyword(s):  
High Temperature ◽  
Ab Initio ◽  
Single Molecule ◽  
Magnetic Relaxation ◽  
Quantitative Prediction ◽  
Relaxation Dynamics ◽  
Efficient Design ◽  
Relaxation Rates ◽  
Design Strategies ◽  
Single Molecule Magnets

<p>Organometallic molecules based on [Dy(Cp<sup>R</sup>)<sub>2</sub>]<sup>+</sup> cations have emerged as clear front-runners in the search for high-temperature single-molecule magnets. However, despite a growing family of structurally-similar molecules, these molecules show significant variations in their magnetic properties, demonstrating the importance of understanding magneto-structural relationships towards developing more efficient design strategies. Here we refine our <i>ab initio</i> spin dynamics methodology and show that it is capable of quantitative prediction of relative relaxation rates in the Orbach region. Applying it to all reported [Dy(Cp<sup>R</sup>)<sub>2</sub>]<sup>+</sup> cations allows us to tease out differences in their relaxation dynamics, highlighting that the main discriminant is the magnitude of the crystal field splitting. We subsequently employ the method to predict relaxation rates for a series of hypothetical organometallic sandwich compounds, revealing an upper limit to the effective barrier to magnetic relaxation of around 2200 K, which has been reached. However, we show that further improvements to single-molecule magnets can be made by moving vibrational modes off-resonance with electronic excitations.</p>

scholarly journals Ab Initio Prediction of High-Temperature Magnetic Relaxation Rates in Single-Molecule Magnets

2021 ◽  
Author(s):  
Daniel Reta ◽  
Jon G. C. Kragskow ◽  
Nicholas Chilton
Keyword(s):  
High Temperature ◽  
Ab Initio ◽  
Single Molecule ◽  
Magnetic Relaxation ◽  
Quantitative Prediction ◽  
Relaxation Dynamics ◽  
Efficient Design ◽  
Relaxation Rates ◽  
Design Strategies ◽  
Single Molecule Magnets

<p>Organometallic molecules based on [Dy(Cp<sup>R</sup>)<sub>2</sub>]<sup>+</sup> cations have emerged as clear front-runners in the search for high-temperature single-molecule magnets. However, despite a growing family of structurally-similar molecules, these molecules show significant variations in their magnetic properties, demonstrating the importance of understanding magneto-structural relationships towards developing more efficient design strategies. Here we refine our <i>ab initio</i> spin dynamics methodology and show that it is capable of quantitative prediction of relative relaxation rates in the Orbach region. Applying it to all reported [Dy(Cp<sup>R</sup>)<sub>2</sub>]<sup>+</sup> cations allows us to tease out differences in their relaxation dynamics, highlighting that the main discriminant is the magnitude of the crystal field splitting. We subsequently employ the method to predict relaxation rates for a series of hypothetical organometallic sandwich compounds, revealing an upper limit to the effective barrier to magnetic relaxation of around 2200 K, which has been reached. However, we show that further improvements to single-molecule magnets can be made by moving vibrational modes off-resonance with electronic excitations.</p>

Magnetic anisotropy on demand exploiting high-pressure as remote control: an ab initio proof-of-concept

2021 ◽  
Author(s):  
Matteo Briganti ◽  
Federico Totti
Keyword(s):  
High Pressure ◽  
High Temperature ◽  
Remote Control ◽  
Magnetic Anisotropy ◽  
Ab Initio ◽  
Single Molecule ◽  
Boiling Temperature ◽  
Proof Of Concept ◽  
Single Molecule Magnets ◽  
On Demand

Lanthanide based single molecule magnets have recently become very promising systems for creating single molecule device working at high temperature (nitrogen boiling temperature). However, the variation of direction of the...

Regulating the magnetic dynamics of mononuclear β-diketone Dy(iii) single-molecule magnets through the substitution effect on capping N-donor coligands

2021 ◽  
Vol 50 (6) ◽  
pp. 2102-2111
Author(s):  
Jing Xi ◽  
Xiufang Ma ◽  
Peipei Cen ◽  
Yuewei Wu ◽  
Yi-Quan Zhang ◽  
...  
Keyword(s):  
Ab Initio ◽  
Single Molecule ◽  
Substitution Effect ◽  
Single Molecule Magnets ◽  
Magnetic Dynamics ◽  
Magnetic Investigation

Substituent change modulates the coordination symmetries and magnetic dynamics of five mononuclear β-diketonate-Dy(iii) complexes with capping N-donor coligands, which is studied by the combination of magnetic investigation and ab initio calculation.

Cu(ii)–Dy(iii) and Co(iii)–Dy(iii) based single molecule magnets with multiple slow magnetic relaxation processes in the Cu(ii)–Dy(iii) complex

2015 ◽  
Vol 44 (29) ◽  
pp. 13242-13249 ◽  
Author(s):  
Malay Dolai ◽  
Mahammad Ali ◽  
Ján Titiš ◽  
Roman Boča
Keyword(s):  
Schiff Base ◽  
Single Molecule ◽  
Schiff Base Ligand ◽  
Magnetic Relaxation ◽  
Magnetic Behaviour ◽  
Dinuclear Complexes ◽  
Relaxation Processes ◽  
Single Molecule Magnets ◽  
Slow Magnetic Relaxation

Two CuII–DyIII and CoIII–DyIII dinuclear complexes of a Schiff base ligand (H3L) exhibit single-molecule magnetic behaviour with multiple slow magnetic relaxation processes for the former.

Structural anisotropy of cyanido-bridged {CoII9WV6} single-molecule magnets induced by bidentate ligands: towards the rational enhancement of an energy barrier

2016 ◽  
Vol 52 (26) ◽  
pp. 4772-4775 ◽  
Author(s):  
Szymon Chorazy ◽  
Michał Rams ◽  
Anna Hoczek ◽  
Bernard Czarnecki ◽  
Barbara Sieklucka ◽  
...  
Keyword(s):  
Single Molecule ◽  
Energy Barrier ◽  
Magnetic Relaxation ◽  
Bidentate Ligands ◽  
Single Molecule Magnets ◽  
Structural Anisotropy ◽  
Slow Magnetic Relaxation

{CoII9[WV(CN)8]6} clusters capped by odd and even number of bidentate ligands reveal the improved slow magnetic relaxation due to the significant structural anisotropy.

Strictly linear trinuclear Dy–Ca/Mg–Dy single-molecule magnets: the impact of long-range f–f ferromagnetic interactions on suppressing quantum tunnelling of magnetization leading to slow magnetic relaxation

2017 ◽  
Vol 46 (25) ◽  
pp. 8259-8268 ◽  
Author(s):  
Wan-Ying Zhang ◽  
Yong-Mei Tian ◽  
Hong-Feng Li ◽  
Peng Chen ◽  
Yi-Quan Zhang ◽  
...  
Keyword(s):  
Long Range ◽  
Single Molecule ◽  
Magnetic Relaxation ◽  
Single Molecule Magnets ◽  
Quantum Tunnelling ◽  
Trinuclear Complexes ◽  
Slow Magnetic Relaxation ◽  
Ferromagnetic Interactions ◽  
The Impact

A series of linear trinuclear complexes Ln2M(OQ)8 [Ln(iii) = Dy and Er, M(ii) = Ca and Mg] were structurally and magnetically investigated.

Towards solvent tuning of slow magnetic relaxation and ferroelectric properties in a dysprosium metal–organic framework system

2019 ◽  
Vol 234 (1) ◽  
pp. 33-41
Author(s):  
Lina Zhang ◽  
Shuyan Guan ◽  
Yunchang Fan ◽  
Chenxia Du ◽  
Dan Zhao ◽  
...  
Keyword(s):  
Single Crystal ◽  
Single Molecule ◽  
Magnetic Relaxation ◽  
Metal Organic Framework ◽  
Ferroelectric Properties ◽  
Relaxation Rates ◽  
Slow Magnetic Relaxation ◽  
Metal Organic ◽  
Solvent Molecules ◽  
Organic Framework

Abstract A new dysprosium metal–organic framework {[Dy2(L)3(H2O)4]·(acetone)2·(H2O)3}n (Dy2-Acetone) with single-molecule magnet and ferroelectric properties was synthesized through a solvent-induced single-crystal-to-single-crystal (SCSC) transformation. Notably, exchange of the coordinated and guest solvent molecules lead to different magnetic relaxation and ferroelectric properties in the dysprosium MOF system, Dy2-DMF and Dy2-Acetone. Study reveals that the tunable magnetic relaxation behaviors are most likely a result of different local coordination sphere and lattice solvent molecules within the pores which influenced and tuned the relaxation rates of the magnetization. Moreover, disparate polar solvent molecules confined in the MOFs may be the key factors for their different ferroelectric properties.

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