Rational enhancement of the energy barrier of bis(tetrapyrrole) dysprosium SMMs <i>via</i> replacing atom of porphyrin core

Cao, Wei; Chen, Gao; Zhang, Yi‐Quan; Qi, Dongdong; Liu, Tao; Wang, Kang; Duan, Chunying; Gao, Song; Jiang, Jianzhuang

doi:10.1039/c5sc02314a

Cited by 89 publications

(40 citation statements)

References 100 publications

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“…S21, Table S5, ESI †). These results are similar to earlier observations for Dy-O vs. Dy-S substitution 14 suggesting a likely generality of such behaviour in Dy(III) complexes.…”

supporting

confidence: 91%

“…1) which is a S-ligated single-ion magnet with hysteresis loops open up to 7 K and a magnetisation reversal barrier of U eff = 638 K, which is unprecedented in the very small family of S-ligated Dy(III) singleion magnets (see Table 1). [14][15][16][17][18][19][20] Compound 1 was isolated by using the cage-like ligand N-(3,5-di-tert-butyl-2-hydroxybenzyl)-N,N-bis(2-pyridylmethyl)amine (HL ON3 ) (see ESI †). 21 Our synthetic strategy generates one short Dy-O bond, to direct the magnetic anisotropy, 22 and three longer Dy-N bonds.…”

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confidence: 99%

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There is nothing wrong with being soft: using sulfur ligands to increase axiality in a Dy(iii) single-ion magnet

et al. 2020

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“…S21, Table S5, ESI †). These results are similar to earlier observations for Dy-O vs. Dy-S substitution 14 suggesting a likely generality of such behaviour in Dy(III) complexes.…”

supporting

confidence: 91%

mentioning

confidence: 99%

There is nothing wrong with being soft: using sulfur ligands to increase axiality in a Dy(iii) single-ion magnet

et al. 2020

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“…Compounds 45 and 46 display butterfly hysteresis loops in their fielddependent magnetisation at 3 K and 3.5 K, respectively, in contrast to 44, which does not show magnetic hysteresis. DFT calculations suggest the improved SIM behaviour is a result of a reduced charge distribution over the oxygen and sulphur atoms, and increased bond lengths that ultimately diminish repulsive electrostatic potential among the ligands and f-electron clouds, which in turn stabilises the |±15/2 ground state [101]. (48) (Fig.…”

Section: Donor Atomsmentioning

confidence: 99%

Molecular single-ion magnets based on lanthanides and actinides: Design considerations and new advances in the context of quantum technologies

McAdams

Ariciu

Kostopoulos

et al. 2017

Coordination Chemistry Reviews

309

226

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Over the past fifteen years or so, the study of f-element single-ion magnets (f-SIMs) has gone from being a sub-discipline of molecular magnetism to an established field of research in its own right. The major driving force has been their exceptional promise in applications such as ultra-high-density data storage, spintronics, and quantum information processing (QIP). Recent demonstrations that f-SIMs preserve their intrinsic magnetic properties even when deposited onto substrates have reinforced the interests in the field.Here, we review the current state of the field of lanthanide and actinide f-SIMs; discuss the principal factors affecting the magnetic and quantum properties of such single-ion magnets; review the latest chemical approaches in designing f-SIMs with superior properties; and highlight new trends in single molecule magnetism, including using f-SIMs as potential spin qubits for quantum computers.

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“…self-assembly building block due to its highly symmetric molecular structure, high flexibility of modification, and strong intermolecular π-π interactions. 23,24 Because of these unique advantages, phthalocyanine shows potential in an extremely wide range of applications, such as organic semiconductors, 25 single-molecule magnets, 26 green catalysts, 27 and phototherapeutic agents. 28,29 On the other hand, the conjugated peptide diphenylalanine is a natural amphiphilic motif that has remarkable biological functions and is able to tune the assembly of various functional molecules to obtain nanomaterials with controllable morphology and considerable stability in an aqueous medium.…”

mentioning

confidence: 99%

Kinetically Controlled Self-Assembly of Phthalocyanine–Peptide Conjugate Nanofibrils Enabling Superlarge Redshifted Absorption

Zhao¹,

Li²,

Liu³

et al. 2019

CCS Chem

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Supramolecular assembly could in principle lead to redshifted absorption through J-aggregation of chromophores, which would be a highly promising method for achieving near-infrared materials with improved functionality and flexibility. To effectively enhance the material functionalities, one of the great challenges remaining is to achieve an aggregation state with a redshift larger than 100 nm. Conventional assemblies that are mostly thermodynamically controlled have a limited redshifted absorption of less than 30 nm. In this work, using a model phthalocyanine–peptide conjugate compound, we achieved the first fabrication of phthalocyanine-based near-infrared materials with a superlarge absorption redshift of 105 nm by a kinetically controlled self-assembly strategy. In this kinetically controlled self-assembly process, sufficient rearrangement of intermolecular aggregates to an ordered structure is revealed to be crucial to facilitate the formation of nanofibrils instead of nanoparticles, which are formed via a general rapid self-assembly pathway under thermodynamic control. The superlarge redshift in the absorbance of assembled nanofibrils originates from the orderly stacked phthalocyanine chromophores, which enable a charge transfer state through more effective intermolecular orbital overlapping. The kinetically controlled J-aggregation state of the phthalocyanine–peptide conjugate with superlarge redshifted absorption not only opens an unprecedented route toward novel near-infrared phthalocyanine materials but also holds great promise for revealing general design principles for various organic dye materials.

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Rational enhancement of the energy barrier of bis(tetrapyrrole) dysprosium SMMs via replacing atom of porphyrin core

Abstract: Replacing a porphyrin N atom induces higher electrostatic environment anisotropy around the Dy center, giving the highest energy barrier among bis(tetrapyrrole) Dy SMMs.

Cited by 89 publications

References 100 publications

There is nothing wrong with being soft: using sulfur ligands to increase axiality in a Dy(iii) single-ion magnet

There is nothing wrong with being soft: using sulfur ligands to increase axiality in a Dy(iii) single-ion magnet

Molecular single-ion magnets based on lanthanides and actinides: Design considerations and new advances in the context of quantum technologies

Kinetically Controlled Self-Assembly of Phthalocyanine–Peptide Conjugate Nanofibrils Enabling Superlarge Redshifted Absorption

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