By changing the counterions (ClO4- and CF3SO3-) and the coordination anions (Cl- and Br-), we investigated their influences on the structures and performances of a class of Zn2Dy chiral single-molecule magnets (SMMs), which are based on a pair of chiral Schiff bases R,R-H2LSchiff and S,S-H2LSchiff {R,R-H2LSchiff = 2-((E)-((1R,2R)-2-((E)-2-hydroxy-3-methoxybenzylideneamino)cyclohexylimino)methyl)-6-methoxyphenol and S,S-H2LSchiff = 2-((E)-((1S,2S)-2-((E)-2-hydroxy-3-methoxybenzylideneamino)cyclohexylimino)methyl)-6-methoxyphenol}. Three pairs of chiral Zn2Dy Schiff base complexes were obtained by directed synthesis, which are [DyZn2(R,R-LSchiff)Cl2(H2O)](ClO4)·0.5MeOH·0.25H2O (R-1) and [DyZn2(S,S-LSchiff)Cl2(H2O)][DyZn2(S,S-LSchiff)Cl2(MeOH)](ClO4)2·MeOH·0.5H2O (S-1), [DyZn2(R,R-LSchiff)Cl2(H2O)](CF3SO3)·0.5MeOH (R-2) and [DyZn2(S,S-LSchiff)Cl2(H2O)][DyZn2(S,S-LSchiff)Cl2(MeOH)](CF3SO3)2·MeOH (S-2), and [DyZn2(R,R-LSchiff)Br2(H2O)](CF3SO3)·0.25MeOH (R-3) and [DyZn2(S,S-LSchiff)Br2(H2O)][DyZn2(S,S-LSchiff)Br2(MeOH)](CF3SO3)2 (S-3). They all exhibit good SMM behaviors, and their magnet relaxation is regulated by not only the counterions (ClO4- and CF3SO3-) but also the coordination anions (Cl- and Br-); these anions also have important effects on the second-harmonic generation (SHG) and third harmonic generation (THG) nonlinear optical properties. Interestingly, in the S-configuration complexes, the coordination solvent molecule of the Dy3+ ion on half of the molecules is the methanol molecule instead of the water molecule. This change in the coordinating solvent molecule can also significantly affect the SMM behaviors and the SHG and THG nonlinear optical properties. Moreover, ab initio calculations were applied to rationally explain the SMM properties.

Effects of Counterions, Coordination Anions, and Coordination Solvent Molecules on Single-Molecule Magnetic Behaviors and Nonlinear Optical Properties of Chiral Zn2Dy Schiff Base Complexes.

The behavior of coordination polymers (CPs) against external stimuli has witnessed remarkable attention, especially when the resulting CPs present reversible molecular arrays. Accordingly, CPs with these characteristics can lead to differences in their properties owing to these structural differences, being promising for their use as potential molecular switches with diverse applications. Herein, we have synthesized four Zn(II) CPs bearing α-acetamidocinnamic acid (HACA) and 4,4′-bipyridine (4,4′-bipy). The reaction between Zn(OAc)2·2H2O, HACA, and 4,4′-bipy yields {[Zn(ACA)2(4,4′-bipy)]·EtOH}n (1), which was used for the formation of three CPs through dissolution–recrystallization structural transformations (DRSTs): {[Zn(ACA)2(4,4′-bipy)]·2MeOH}n (2), {[Zn2(μ-ACA)2(ACA)2(4,4′-bipy)]·2H2O}n (3), and {[Zn3(μ-ACA)6(4,4′-bipy)]·0.75CHCl3}n (4). The study of the four crystal structures revealed that their secondary building units (SBUs) comprise monomeric, dimeric, and trimeric arrangements linked by 4,4′-bipy ligands. The fundamental role of the utilized solvent and/or temperature, as well as their effect on the orientation of the amide moieties driving the formation of the different SBUs is discussed. Furthermore, the reversibility and interconversion between the four CPs have been assayed. Finally, their solid-state photoluminescence has evinced that the effect of the amide moieties not only predetermine a different SBU but also lead to a different emission in 4 compared with 1–3.

/pdf/amide-driven-secondary-building-unit-structural-14n6aecm.pdf

Amide-Driven Secondary Building Unit Structural Transformations between Zn(II) Coordination Polymers

Since the last century, we have witnessed the development of molecular magnetism which deals with magnetic materials based on molecular species, i.e., organic radicals and metal complexes. Among them, the broadest attention was devoted to molecule-based ferro-/ferrimagnets, spin transition materials, including those exploring electron transfer, molecular nanomagnets, such as single-molecule magnets (SMMs), molecular qubits, and stimuli-responsive magnetic materials. Their physical properties open the application horizons in sensors, data storage, spintronics, and quantum computation. It was found that various optical phenomena, such as thermochromism, photoswitching of magnetic and optical characteristics, luminescence, nonlinear optical and chiroptical effects, as well as optical responsivity to external stimuli, can be implemented into molecule-based magnetic materials. Moreover, the fruitful interactions of these optical effects with magnetism in molecule-based materials can provide new physical cross-effects and multifunctionality, enriching the applications in optical, electronic, and magnetic devices. This Review aims to show the scope of optical phenomena generated in molecule-based magnetic materials, including the recent advances in such areas as high-temperature photomagnetism, optical thermometry utilizing SMMs, optical addressability of molecular qubits, magneto-chiral dichroism, and opto-magneto-electric multifunctionality. These findings are discussed in the context of the types of optical phenomena accessible for various classes of molecule-based magnetic materials.

Optical Phenomena in Molecule-Based Magnetic Materials

Chiral lanthanide clusters provide a platform for molecular-based materials with coordination between chirality and magnetism, and exhibited great application prospects in the fields of three-dimensional displays, magneto-optical memories, and spintronic...

Coordination site manipulation of annular growth mechanism to assemble chiral lanthanide clusters with different shapes and magnetic properties

Single-molecule magnets (SMMs) show wide potential applications in the field of ultrahigh-density storage materials, quantum computing, spintronics, and so on. Lanthanide (Ln) SMMs, as an important category of SMMs, open up a promising prospect due to their large magnetic moments and huge magnetic anisotropy. However, the construction of high performance for Ln SMMs remains an enormous challenge. Although remarkable advances are focused on the topic of Ln SMMs, the research on Ln SMMs with different nuclear numbers is still deficient. Therefore, this review summarizes the design strategies for the construction of Ln SMMs, as well as the metal skeleton types. Furthermore, we collect reported Ln SMMs with mononuclearity, dinuclearity, and multinuclearity (three or more Ln spin centers) and the SMM properties including energy barrier (Ueff) and pre-exponential factor (τ0) are described. Finally, Ln SMMs with low-nuclearity SMMs, especially for single-ion magnets (SIMs), are highlighted to understand the correlations between structures and magnetic behavior of the detail SMM properties are described. We expect the review can shed light on the future developments of high performance Ln SMMs.

Lanthanide single-molecule magnets: synthetic strategy, structures, properties and recent advance.

By the bridging action of the 6-chloro-2-hydroxypyridine (Hchp) ligand and the terminal coordination role of the homochiral ligand, (-)/(+)-3-trifluoroacetyl camphor (l-Htfc/d-Htfc), a pair of enantiomerically pure dysprosium(III) dinuclear complexes, [Dy2(l-tfc)4(chp)2(MeOH)2] (l-1) and [Dy2(d-tfc)4(chp)2(MeOH)2] (d-1), was obtained. Their circular dichroism (CD) spectra verified their enantiomeric nature. Magnetic investigation indicated that they exhibit ferromagnetic interaction and good zero field single-molecule magnet (SMM) properties. The Ueff/k values of l-1 and d-1 at 0 Oe are 180.5 and 181.3 K, respectively, which are large values for homochiral Dy(III) SMMs. A reasonable explanation for the magnetic properties of l-1 and d-1 was supplied by ab initio calculations. Remarkably, magnetic circular dichroism (MCD) investigation revealed that the chiral Dy2 enantiomers show a strong magneto-optical Faraday effect at room temperature, suggesting potential applications in magneto-optical devices.

Homochiral Ferromagnetic Coupling Dy2 Single-Molecule Magnets with Strong Magneto-Optical Faraday Effects at Room Temperature.

Mechanochromic luminescent materials have attracted considerable attention because of their interesting color switching behavior under mechanical grinding or hydrostatic pressure. Here, the intrigu...

Mechanochromic and Single-Molecule Magnetic Properties of a Rhodamine 6G Dy(III) Complex

Chiral Co-Crystals of (S)- or (R)-1,1′-Binaphthalene-2,2′-diol and Zn2Dy2 Tetranuclear Complexes Behaving as Single-Molecule Magnets

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Homochiral Ferromagnetic Coupling Dy2 Single-Molecule Magnets with Strong Magneto-Optical Faraday Effects at Room Temperature.

Mechanochromic and Single-Molecule Magnetic Properties of a Rhodamine 6G Dy(III) Complex

Chiral Co-Crystals of (S)- or (R)-1,1′-Binaphthalene-2,2′-diol and Zn2Dy2 Tetranuclear Complexes Behaving as Single-Molecule Magnets